Swirl nozzles, pipe distributors, fluidized bed reaction apparatus, and methods for hydrocarbon ammoxidation reactions

Abstract

The present application relates to the technical fields of chemical equipment, and discloses a cyclone nozzle, a tubular distributor, a fluidized bed reaction device and a hydrocarbon ammoxidation reaction method. The cyclone nozzle comprises a shell, the shell is formed around a cyclone cavity, the cyclone cavity comprises an upper cyclone cavity and a lower cyclone cavity, a bottom end of the lower cyclone cavity is formed with a bottom end opening, and the shell is provided with a nozzle feed port communicating with the upper cyclone cavity; a center column is arranged in the cyclone cavity, a bottom end of the center column extends to the bottom end opening of the lower cyclone cavity, and the bottom end of the center column is connected with a flow guide body, and a nozzle discharge port in the form of an annular gap is formed between the flow guide body, the bottom end of the center column and the bottom end opening of the lower cyclone cavity. The present application can strengthen the uniform gas distribution performance of the tubular distributor, and further improve the yield of ammoxidation products.

Description

Technical Field

[0001] This invention relates to the field of chemical equipment technology, specifically to a swirl nozzle, a tubular distributor, a fluidized bed reactor, and a method for hydrocarbon ammonia oxidation reaction. Background Technology

[0002] Tubular distributors are a type of gas distributor widely used in catalytic cracking and hydrocarbon ammonia oxidation reactors. They are characterized by having a free end, which helps address issues related to thermal expansion and multi-stage gas feeding, making them particularly suitable for large reactors and processes requiring multiple gas feeds. Currently, tubular distributors consist of a main pipe, branch pipes, sub-branch pipes, and nozzles.

[0003] CN204017797U discloses a feed distributor for an ammonia oxidation reactor. Different sections of the feed distributor, used in commercial ammonia oxidation reactors, are easily replaced by attaching the various sections of the distributor to each other and to the reactor wall using airtight quick-disconnect fittings. Furthermore, the diameters of the branch pipes and the feed nozzles attached to these branch pipes are varied within these distributor sections to facilitate uniform flow of the feed gas through these components. The distributor can be subdivided into multiple feed distributor sections arranged for better reactor control. Finally, end caps terminating at the distal ends of the distributor branch pipes may be equipped with nozzles to remove any ammonia oxidation catalyst that may unintentionally reach the interior of the distributor. However, as reactor size increases, the problem of non-uniform flow field within the distributor worsens. Summary of the Invention

[0004] Existing tubular distributor nozzles are mostly simple short pipes connected to branch pipes. When the gas flow enters the nozzle from the branch pipe, the drastic change in flow direction leads to severe flow deviation, and even backflow of substances outside the tubular distributor (such as catalysts) due to local decompression. While pressure swirl nozzles, commonly used in liquid atomization, have good uniform distribution performance, they generate strong backflow due to central centrifugal decompression, making them difficult to apply in reactors containing particulate materials (such as catalyst particles). Furthermore, they are also difficult to apply in hydrocarbon ammonia oxidation reactions, which often employ tubular distributors. Based on the foregoing, the purpose of this invention is to overcome the problems existing in the prior art. Through extensive CFD simulations, flow field analysis, and specific experimental studies, this invention provides a swirl nozzle, tubular distributor, fluidized bed reactor, and method for hydrocarbon ammonia oxidation reactions. This method can enhance the uniform gas distribution performance of the tubular distributor and further improve the yield of ammonia oxidation products.

[0005] To achieve the above objectives, the present invention provides a swirling nozzle, the swirling nozzle comprising:

[0006] A housing, the housing surrounding a swirling cavity, the swirling cavity including an upper swirling cavity and a lower swirling cavity, the bottom end of the lower swirling cavity having a bottom opening, and the housing being provided with a nozzle inlet communicating with the upper swirling cavity;

[0007] A central column is disposed in the swirling cavity. The top end of the central column is connected to the top wall of the shell of the swirling cavity, and the bottom end of the central column extends toward the bottom opening of the lower swirling cavity. A guide fluid is connected to the bottom end of the central column, and a nozzle outlet with an annular gap is formed between the guide fluid, the bottom end of the central column, and the bottom opening of the lower swirling cavity.

[0008] The material entering from the nozzle inlet can flow along the inner wall of the swirling chamber to form a downward swirling flow around the central column, and the downward swirling flow is ejected in an umbrella shape through the nozzle outlet.

[0009] A second aspect of the present invention provides a tubular distributor, the tubular distributor comprising a branch pipe and multiple branch pipes connected to the branch pipe, the branch pipes being equipped with multiple swirling nozzles as described in the present invention, and the connection end between the branch pipes and the branch pipes being provided with a rectifier capable of enhancing material distribution.

[0010] A third aspect of the present invention provides a fluidized bed reactor, the fluidized bed reactor having a reaction chamber, wherein a material distributor is disposed in the reaction chamber, the material distributor including the tubular distributor described in the present invention.

[0011] The fourth aspect of the present invention provides the application of the swirl nozzle, the tubular distributor, or the fluidized bed reactor described in the present invention in ammonia oxidation, catalytic cracking, nitrobenzene hydrogenation, or coal gasification reactions.

[0012] The fifth aspect of the present invention provides a method for ammonia oxidation reaction of hydrocarbons, the method employing the fluidized bed reactor described in the present invention, wherein the material distributor includes at least one tubular distributor and a gas distribution plate described in the present invention;

[0013] Preferably, the method includes:

[0014] Raw materials containing hydrocarbon and ammonia sources enter the reaction chamber through the tubular distributor.

[0015] Oxygen-containing gas enters the reaction chamber through a gas distribution plate;

[0016] Within the reaction chamber, raw materials containing hydrocarbon and ammonia sources react with oxygen-containing gas. Preferably, the raw materials containing hydrocarbon and ammonia sources react with oxygen-containing gas in a counter-current manner.

[0017] Through the above technical solutions, the swirling nozzle of the present invention enables the incoming material to flow along the inner circumferential wall of the swirling chamber to form a downward swirling flow around the central column, and is ejected in an umbrella shape through the nozzle outlet. On the one hand, it can achieve a more optimized material flow distribution effect, and on the other hand, it can eliminate the influence of backflow of material outside the swirling nozzle caused by local pressure reduction. The rectifier component of the tubular distributor of the present invention can eliminate gas deviation inside the tubular distributor, making the gas distribution performance of the distributor closer to the ideal gas distribution state, and enhancing the uniform distribution of airflow. Furthermore, it makes the reactants in the fluidized bed reactor of the present invention closer to the ideal gas distribution state, allowing the reactants to fully contact and improving the raw material conversion rate. Furthermore, it makes the method of hydrocarbon ammonia oxidation reaction of the present invention have the effect of improving the yield of ammonia oxidation products and reducing the amount of raw materials used. Attached Figure Description

[0018] Figure 1 This is a schematic diagram of a fluidized bed reactor according to a specific embodiment of the present invention;

[0019] Figure 2 yes Figure 1 A schematic diagram of a center-tube distributor;

[0020] Figure 3 yes Figure 2 Schematic diagram of the structure of the central branch pipe-branch pipe;

[0021] Figure 4 yes Figure 2 A schematic diagram of one type of branch pipe;

[0022] Figure 5 yes Figure 2 A schematic diagram of another form of branch pipe;

[0023] Figure 6 yes Figure 2 Schematic diagram of the connection between the central branch pipe and the branch pipe (top view);

[0024] Figure 7 yes Figure 2 A three-dimensional structural diagram of a vortex nozzle;

[0025] Figure 8 This is a schematic diagram of the longitudinal section of a swirling nozzle;

[0026] Figure 9 This is a schematic diagram of the cross-sectional structure of a swirling nozzle at the nozzle inlet.

[0027] Figure 10 This is a schematic diagram of the structure of a tubular distributor in the prior art;

[0028] Figure 11This is a comparison diagram of the flow distribution of the distributor using variable diameter and rectifier components in this invention and a conventional distributor.

[0029] Explanation of reference numerals in the attached figures

[0030] 1 is the gas collecting chamber; 2 is the reaction chamber; 3 is the heat exchange device; 4 is the tubular distributor; 5 is the hydrocarbon source; 6 is the ammonia source; 7 is the gas distribution plate; 8 is the oxygen-containing gas; 9 is the second material inlet; 10 is the cyclone separator; 11 is the first material outlet; 12 is the main pipe; 13 is the branch pipe; 14 is the branch pipe; 15 is the main flow direction; 16 is the rectifier component; 17 is the straight tube shell; 18 is the curved tube shell with different diameters; 19 is the swirl nozzle; 20 is the incoming gas in the branch pipe; 21 is the nozzle inlet; 22 is the upper swirl chamber; 23 is the lower swirl chamber; 24 is the central column; 25 is the nozzle outlet; 26 is the guide fluid; 211 is the first inner wall. Detailed Implementation

[0031] The specific embodiments of the present invention will be described in detail below with reference to the accompanying drawings. It should be understood that the specific embodiments described herein are for illustration and explanation only and are not intended to limit the present invention.

[0032] The endpoints and any values ​​of the ranges disclosed herein are not limited to the precise ranges or values, and these ranges or values ​​should be understood to include values ​​close to these ranges or values. For numerical ranges, the endpoint values ​​of the various ranges, the endpoint values ​​of the various ranges and individual point values, and individual point values ​​can be combined with each other to obtain one or more new numerical ranges, which should be considered as specifically disclosed herein.

[0033] In this invention, unless otherwise stated, directional terms such as "upper," "lower," "top," and "bottom" are generally used to describe the relative positions of components in relation to the directions shown in the accompanying drawings or in relation to the vertical, perpendicular, or gravitational directions; "inner" and "outer" generally refer to the interior or exterior of the cavity relative to the inner chamber or the radial interior or exterior relative to the center of the circle.

[0034] like Figures 7-8 As shown, the first aspect of the present invention provides a swirling nozzle, the swirling nozzle 19 comprising:

[0035] The shell has a swirling cavity formed around it. The swirling cavity includes an upper swirling cavity 22 and a lower swirling cavity 23. The lower swirling cavity 23 is configured as a tapered cavity that tapers downwards. The bottom end of the tapered cavity has a bottom opening. The shell is provided with a nozzle inlet 21 that communicates with the upper swirling cavity 22.

[0036] A central column 24 is disposed in the swirling chamber. The top end of the central column 24 is connected to the top wall of the swirling chamber shell, and the bottom end of the central column 24 extends into the bottom opening of the lower swirling chamber 23. A guide fluid 26 is connected to the bottom end of the central column 24. A nozzle outlet 25 with an annular gap is formed between the guide fluid 26, the bottom end of the central column 24, and the bottom opening of the lower swirling chamber 23. Thus, if... Figure 8 As shown, the entire shell is essentially fitted around the central column 24 and the fluid guide 26, but does not come into contact with the fluid guide 26.

[0037] The material entering from the nozzle inlet 21 can flow along the inner wall of the swirling chamber to form a downward swirling flow around the central column 24. The downward swirling flow is sprayed out in an umbrella shape through the nozzle outlet 25. This achieves a more optimized material flow distribution effect on the one hand, and eliminates the backflow of substances (such as catalysts) outside the swirling nozzle due to local pressure reduction on the other hand.

[0038] like Figure 8 As shown, according to a preferred embodiment of the present invention, the guide fluid 26 includes a gradually expanding section with a cross-section that gradually increases in size along the axial direction. The small end of the gradually expanding section is connected to the bottom end of the central column 24, and the cross-sectional area of ​​the large end of the gradually expanding section is larger than the area of ​​the bottom opening of the lower swirling cavity 23.

[0039] It should be noted that the material backflowed into the swirl nozzle 19 in this invention is exemplified by catalyst particles, but the invention is not limited to this. In some embodiments of the fluidized bed reactor, the catalyst particles are carried upward by the bottom feed gas (e.g., air), and the nozzle outlet 25 of the swirl nozzle 19 is located above the bottom feed gas inlet, and the nozzle outlet 25 faces the bottom of the fluidized bed reactor. In this way, due to the higher gas velocity at the nozzle outlet 25, local decompression is formed, which causes the catalyst particles carried upward with the gas to be sucked into the swirl nozzle, while the guide fluid 26 can prevent the backflow of catalyst. Furthermore, the guide fluid 26 is configured as a frustum shape, with the small end of the frustum connected to the bottom end of the central column 24. The connection surface between the two can be located above, below, or flush with the bottom end face of the conical cavity. The distance in the height direction between the connection surface of the guide fluid 26 and the bottom end face of the conical cavity is 0 to 0.1 times the diameter of the central column 24.

[0040] In this invention, the central column 24 can be a cylinder of equal diameter or a conical column with a diameter that gradually decreases from top to bottom, and the ratio of the diameter of the large end to the diameter of the small end of the conical column is 1 to 1.5.

[0041] According to a preferred embodiment of the present invention, a tapering section with a gradually decreasing cross-section along the axial direction is provided below the expanding section; the tapering section is set in a conical shape, so that when the gas fed from below the swirl nozzle 19 carries particulate matter, such as catalyst particles, and passes through the conical tapering section upward, the catalyst particles are dispersed, which increases the contact area with the reactants on the one hand, and the dispersed catalyst is also moved away from the nozzle outlet 25, thereby avoiding being sucked into the nozzle due to pressure difference.

[0042] According to a preferred embodiment of the present invention, the converging section and the expanding section are connected by a buffer section. The converging section, the buffer section, and the expanding section can be integrally formed. The buffer section is cylindrical or drum-shaped with a raised center, so that the longitudinal cross-section of the guide fluid 26 is approximately elliptical or spindle-shaped. The buffer section in the middle increases the distance between the converging section and the expanding section, so that the particles dispersed by the conical converging section can be further away from the nozzle outlet 25 when they reach the height of the nozzle outlet 25 to avoid being sucked into the nozzle 19, thereby eliminating the effect of backflow.

[0043] In this invention, the nozzle inlet 21 is connected to the peripheral wall of the housing and communicates with the upper swirling cavity 22. The nozzle inlet 21 extends along the tangential direction, involute direction, or helical direction of the inner peripheral wall of the housing, so that the material is fed along one of the tangential, involute, or helical directions of the swirling cavity 22; for example... Figure 7 As shown, in some embodiments of the present invention, the nozzle inlet 21 extends along the tangential direction of the inner peripheral wall of the housing.

[0044] In this invention, such as Figure 9 As shown, the line connecting the intersection of the first inner wall 211 of the nozzle inlet 21 and the inner peripheral wall of the housing with the center of the housing has an angle β of 60° to 120° with the tangent at the intersection.

[0045] In this invention, the normal cross-section of the material flow direction of the nozzle inlet 21 is one of a rectangle, a circle, or an ellipse.

[0046] In this invention, the upper swirling cavity 22 is a cylindrical or frustum-shaped cavity.

[0047] In this invention, the ratio of the height of the cylindrical cavity and / or the frustum-shaped cavity to the diameter of the circle at the middle position is preferably 0.1 to 10.

[0048] In this invention, it is more preferable that the ratio of the maximum diameter to the minimum diameter of the frustum-shaped cavity is 0.1 to 10.

[0049] In this invention, the top diameter of the conical cavity is the same as the bottom diameter of the upper swirling cavity 22, and the ratio of the bottom diameter to the top diameter of the conical cavity is 0.1 to 10. It should be noted that the lower swirling cavity of the nozzle in this invention is not limited to... Figures 7-8The downwardly tapered cavity shown can also be a downwardly expanding tapered cavity depending on the actual usage requirements. In the embodiments of the present invention, the downwardly tapered cavity is only used as an example to illustrate the advantages of the present invention, but the present invention is not limited to this.

[0050] like Figures 4-6 As shown, a second aspect of the present invention provides a tubular distributor 4, including a branch pipe 13 and multiple branch pipes 14 connected to the branch pipe 13. Multiple swirling nozzles 19 of the present invention are installed on the branch pipes 14. A flow-rectifying member 16 is provided at the connection end between the branch pipes 14 and the branch pipes 13. This eliminates gas flow deviation inside the tubular distributor 4, thereby enhancing the uniform distribution of airflow. Figure 11 As shown, CFD analysis indicates that the above-mentioned components can significantly suppress flow deviation and turbulence within the distributor, thereby enhancing the uniform distribution of flow.

[0051] In this invention, such as Figure 3 As shown, the tubular distributor 4 is a tree-shaped tubular distribution structure; multiple branch pipes 14 are arranged on both sides of the branch pipe 13, and the multiple branch pipes 14 on both sides are arranged symmetrically about the branch pipe 13, and the length gradually decreases from the middle of the branch pipe toward both ends.

[0052] In this invention, the branch pipe 14 extends radially along the branch pipe 13, one end of the branch pipe 14 is connected to the side of the branch pipe 13 through the rectifier 16, and the other end is closed; the cross-section of the branch pipe 14 is circular, elliptical or rectangular.

[0053] According to a preferred embodiment of the present invention, along the main flow direction 15, the branch pipe 13 is a tapered pipe with a gradually decreasing cross-sectional area; this allows for a uniform distribution of the gas flow rate entering the branch pipe 14 from the branch pipe 13. Further, it is preferable that the branch pipe 13 is a circular pipe, with the ratio of the large end diameter to the small end diameter being 0.1 to 0.9; more preferably, the branch pipe 13 is composed of multiple circular pipe segments of different diameters connected end-to-end; further preferably, the length of each segment accounts for 0.05 to 0.95 of the total length of the branch pipe 13; further preferably, the ratio of the maximum diameter to the minimum diameter of the branch pipe 13 is 0.1 to 0.9. Figure 2 As shown, in this invention, the tubular distributor 4 also includes a main pipe 12 and multiple branch pipes 13, which are arranged radially on the side of the main pipe 12. One end of each branch pipe 13 is connected to the main pipe 12, and the other end is closed.

[0054] It should be noted that by adding a main pipe 12 and multiple branch pipes 13, the gaseous raw material enters from the main pipe 12, is then distributed to the multiple branch pipes 13, and finally distributed to all the branch pipes 14. This can greatly increase the ventilation capacity, increase the chemical reaction output, and help reduce the unit cost of the equipment operation and improve economic efficiency.

[0055] According to a preferred embodiment of the present invention, the rectifier 16 is a section of pipe with a variable diameter, such as... Figures 4-6 As shown, the large end of the rectifier 16 is connected to the radial direction of the branch pipe 13, and the small end is connected to the branch pipe 14. The rectifier 16 and the branch pipe can have various shapes, such as... Figure 4 or Figure 5 As shown, the flow cross-section of the rectifier component 16 is circular, elliptical, or rectangular to connect to the corresponding circular or square tube branch pipe. In this embodiment of the invention, a circular tube branch pipe is used as an example to illustrate the advantages of the invention, but the invention is not limited thereto.

[0056] According to a preferred embodiment of the present invention, the shell surrounding the rectifying member 16 can be considered axially as being composed of a straight shell 17 and a curved shell 18 with varying diameters. That is, the straight shell 17 and the curved shell 18 located below the straight shell 17 together form the variable diameter cavity of the rectifying member 16. The radial cross-section of the curved shell 18 with its center at the top is an inwardly concave arc shape. The diameter of the inwardly concave arc shape gradually decreases along the flow direction inside the rectifying member 16 until the cross-sectional area of ​​the cavity formed by the straight shell 17 is the same as the cross-sectional area of ​​the branch pipe 14. Specifically, viewed from the longitudinal cross-section of the rectifying member 16, the profile of the curved shell 18 along the flow direction inside the rectifying member 16 is one of a circular arc, an elliptical arc, or a parabola. The straight shell 17 and the curved shell 18 are smoothly connected radially to reduce the resistance of the airflow flowing through the rectifying member 16.

[0057] According to a preferred embodiment of the present invention, the angle α between the outer contour of the straight tube shell 17 and the main flow direction 15 of the branch pipe 13 is 90° to 175°; along the flow direction within the rectifying member 16, the profile of the variable diameter curved tube shell 18 is one of a circular arc, an elliptical arc, or a parabola.

[0058] A third aspect of the present invention provides a fluidized bed reactor, the fluidized bed reactor having a reaction chamber 2, and a material distributor being provided in the reaction chamber 2, the material distributor including the tubular distributor 4 of the present invention.

[0059] In this invention, preferably, the material distributor includes at least one tubular distributor 4 and a gas distribution plate 7; more preferably, the ratio of the vertical distance between the gas distribution plate 7 and the adjacent tubular distributor 4 to the height of the reaction chamber 2 is 0.01 to 0.1.

[0060] The fluidized bed reactor of the present invention is applied in ammonia oxidation reaction, and also includes some structures found in conventional ammonia oxidation reactors in the prior art, such as gas collecting chambers, cyclone separators, and heat exchangers. Specifically, for example, in some embodiments of the present invention, such as... Figure 1As shown, the fluidized bed reactor has a reaction chamber 2 and is equipped with a first material inlet, a second material inlet 9, and a first material outlet 11 connected to the reaction chamber 2. A heat exchange device 3 is installed inside the reaction chamber 2. The first material inlet is connected to the tubular distributor 4 of this invention. Specifically, the first material outlet 11 is located at the top of the fluidized bed reactor, and the second material outlet, equipped with a control valve, is located at the bottom of the fluidized bed reactor. A constriction section is formed at the bottom of the reaction chamber, and the bottom end of the constriction section extends downward to form the second material outlet. The first material outlet 11 is connected to the gas collection chamber 1. The gas collection chamber 1 is connected to the cyclone separator 10. After the product gas from the reaction is separated from the catalyst particles by the cyclone separator 10, it enters the gas collection chamber 1 and is discharged from the first material outlet. In this invention, the first material... The inlet is located below the cyclone separator 10. The first material inlet is connected to the main pipe 12 of the tubular distributor 4, and the nozzle outlet 25 of the cyclone nozzle 19 of the tubular distributor 4 connected to the first material inlet faces the bottom space of the reaction chamber 2. The second material inlet 9 is located below the first material inlet. The second material inlet is a pipe that radially penetrates the cavity wall of the constricted section, and the pipe located in the reaction chamber bends downward. In this way, the gas entering through the second material inlet 9 is reflected by the cavity wall of the constricted section and dispersed upwards again by the gas distribution plate 7 located above the second material inlet 9. The gas distribution plate 7 is located below the tubular distributor 4. In this way, the material from the first material inlet and the material from the second material inlet come into countercurrent contact and react fully.

[0061] The fourth aspect of the present invention provides the application of the swirl nozzle, the tubular distributor, or the fluidized bed reactor described in the present invention in hydrocarbon ammonia oxidation, catalytic cracking, nitrobenzene hydrogenation, or coal gasification reactions.

[0062] The fifth aspect of the present invention provides a method for ammonia oxidation of hydrocarbons, the method being carried out in a fluidized bed reactor of the present invention, wherein the material distributor includes at least one tubular distributor 4 and a gas distribution plate 7.

[0063] In this invention, preferably, the method includes: raw materials containing hydrocarbon sources and ammonia sources enter the reaction chamber 2 through a tubular distributor 4, and oxygen-containing gas enters the reaction chamber 2 through a gas distribution plate 7; the raw materials containing hydrocarbon sources and ammonia sources react with the oxygen-containing gas in the reaction chamber, preferably, the raw materials containing hydrocarbon sources and ammonia sources react with the oxygen-containing gas in a reverse reaction.

[0064] Raw materials containing hydrocarbon and ammonia sources are sprayed out by the tubular distributor 4 and swirl nozzle 19 of this invention, and then mixed with oxygen-containing gas. Under the action of a catalyst, an ammonia oxidation reaction is carried out, which improves the uniformity of raw material distribution and utilization rate, thereby increasing the yield of ammonia oxidation products.

[0065] In this invention, the non-uniformity of the jet flow rate from the tubular distributor 4 can reach 0–0.35; wherein, the non-uniformity calculation method in this invention is as follows: Where n is the number of swirling nozzles 19, u i The ejection flow rate of the swirl nozzle 19 is... The average flow rate of the swirling nozzle 19 is, for example, n can be 200-5000.

[0066] In this invention, during specific implementation, only the main inlet flow rate is controlled (generally controlled at 5 × 10). -3 -80m 3 / h), and through the device of the present invention, the flow rate of each nozzle can be naturally formed. Using the technical solution of the present invention, u i The range is 0-10m 3 / h, The range is 1×10 -6 -0.8m 3 / h. Thus, the non-uniformity of the jet flow rate of the tubular distributor 4 of the present invention can reach 0 to 0.35.

[0067] In this invention, the catalyst is pre-filled above the gas distribution plate 7. The oxygen-containing gas entering from the second material inlet at the bottom carries the catalyst and comes into contact with and mixes with the raw materials containing hydrocarbon source and ammonia source. After the reaction, a nitrile crude product gas is obtained. The nitrile crude product gas enters the cyclone separator 10 to separate the catalyst and then enters the gas collection chamber 1. The catalyst separated from the cyclone separator 10 falls back to the reaction zone bed from the material leg.

[0068] In this invention, the preferred molar ratio of hydrocarbon source (calculated as hydrocarbon group), ammonia source (calculated as amino group), and oxygen-containing gas (calculated as oxygen molecule) is 1:(1-10):(10-40).

[0069] In this invention, the preferred hydrocarbon source includes hydrocarbons and / or hydrocarbon derivatives, and more preferably includes at least one of toluene, p-chlorotoluene, o-chlorotoluene, o-xylene, m-xylene, p-xylene, dichlorotoluene, trichlorotoluene, or 4-nitro-o-xylene.

[0070] In this invention, the ammonia source is selected from ammonia gas or a mixture of gases containing ammonia gas, and the oxygen-containing gas is selected from oxygen gas or a mixture of gases containing oxygen gas, such as air. This invention has no special requirements for the ammonia source and the oxygen-containing gas, and will not be elaborated here.

[0071] In this invention, the preferred contact conditions include: a reaction temperature of 300–500°C, a pressure of 0.01–0.2 MPa, and a gas apparent linear velocity of 0.1–0.8 m / s.

[0072] The catalyst used in this invention is a commonly used catalyst for hydrocarbon ammonia oxidation reaction in the prior art, such as NC-III type or other vanadium-chromium silica supported particle catalysts.

[0073] The present invention is further illustrated below with examples, but the present invention is not limited thereto.

[0074] In this embodiment of the invention, air is used as an example of oxygen-containing gas, ammonia is used as an example of ammonia source, and NC-III type catalyst is used as an example of catalyst (this invention has no special requirements for catalyst, and commonly used catalysts in the art can be applied to this invention).

[0075] The following examples are in Figures 1-8 The fluidized bed reactor shown is used in the reaction. The fluidized bed reactor has a reaction chamber 2, in which a heat exchange device 3 and a tubular distributor 4 are installed. A first material outlet 11 is provided at the top of the reaction chamber, which is connected to a gas collection chamber 1. The gas collection chamber 1 is connected to a cyclone separator 10. A first material inlet connected to the tubular distributor 4 is provided below the cyclone separator 10. The nozzle outlet 25 of the cyclone nozzle 19 faces the bottom space of the reaction chamber 2. A second material inlet 9 is provided below the first material inlet, and a gas distribution plate 7 is provided below the tubular distributor 4.

[0076] The tubular distributor 4 includes a main pipe 12 and multiple branch pipes 13 arranged radially on the side of the main pipe 12. One end of each branch pipe 13 is connected to the main pipe 12, and the other end is closed. Each branch pipe 13 is composed of multiple segments of circular pipes of different diameters connected end to end. Multiple branch pipes 14 extend radially along the branch pipes 13. One end of each branch pipe 14 is connected to the side of the branch pipe 13 through a flow rectifying member 16, and the other end is closed. The flow rectifying member 16 is a pipe with a variable diameter. The large end of the flow rectifying member 16 is connected to the radial direction of the branch pipe 13, and the small end is connected to the branch pipe 14. The shell surrounding the flow rectifying member 16 is composed of a straight shell 17 and a curved shell 18 with different diameters. The straight shell 17 and the curved shell 18 with different diameters are smoothly connected radially. Along the flow direction within the flow rectifying member 16, the profile of the curved shell 18 with different diameters is parabolic.

[0077] The swirling nozzle 19 includes: a housing, around which a swirling cavity is formed, the swirling cavity including an upper swirling cavity 22 and a lower swirling cavity 23, the lower swirling cavity 23 being configured as a downwardly tapered cone cavity with a bottom opening at the bottom end, and a nozzle inlet 21 being provided in the upper swirling cavity; a central column 24 is provided in the swirling cavity, the top end of the central column 24 being connected to the top wall of the housing of the swirling cavity, the bottom end of the central column 24 extending to the bottom opening of the lower swirling cavity 23, the bottom end of the central column 24 being connected to a guide fluid 26, and a nozzle outlet 25 with an annular gap being formed between the guide fluid 26, the bottom end of the central column 24 and the bottom opening of the lower swirling cavity 23; the guide fluid 26 includes, from top to bottom, a frustum-shaped expanding section, a cylindrical buffer section and an inverted conical tapering section, the small end of the frustum-shaped expanding section being connected to the bottom end of the central column 24.

[0078] The method for hydrocarbon ammonia oxidation reaction includes: introducing raw materials containing hydrocarbon source and ammonia source into the first material inlet, and introducing air into the second material inlet; the raw materials containing hydrocarbon source and ammonia source and the air carrying NC-III type catalyst are contacted in the reaction chamber 2 to obtain nitrile crude product gas, the nitrile crude product gas enters the cyclone separator 10 to separate the catalyst and then enters the gas collection chamber 1 and is discharged from the first material outlet 11.

[0079] In the following embodiments 1-6, the tubular distributor 4 has 4 branch pipes 13, 14 branch pipes 14 per branch pipe, and the inlet flow rate of the main pipe 12 is 60m³ / h. 3 / h, all can achieve a non-uniformity of 0 to 0.35 in the jet flow rate of the tubular distributor 4 in Examples 1-6.

[0080] Example 1

[0081] The branch pipe 13 of the tubular distributor 4 is composed of three connected circular pipes of different diameters. Along the flow direction within the pipe, the diameter ratio of the three circular pipes is 1:0.75:0.35, and the corresponding proportions of the three pipes to the total length of the branch pipe 13 are 0.8:0.1:0.1. The branch pipe 14 is connected to the branch pipe 13 via a flow rectifying component 16. The angle α between the outer contour of the straight pipe shell 17 and the main flow direction 15 of the branch pipe 13 is 160°. The outer contour of the flow rectifying component's curved surface is an arc, and the internal flow channel cross-section of the flow rectifying component is elliptical. Swirl-type flow meters are installed at equal intervals on the branch pipe 14. The nozzle has an inlet 21 that extends along the involute direction of the inner circumferential wall of the shell, has a square cross-section, and an included angle β of 60°. The upper cylindrical swirling cavity of the nozzle has the same height and diameter, and the top diameter of the lower swirling conical cavity is the same as the bottom diameter of the upper swirling cavity. The ratio of the bottom diameter to the top diameter is 0.25. The central column 24 of the swirling nozzle is a cylinder of equal diameter. The connection surface between the central column of the swirling nozzle and the guide fluid is flush with the lower end face of the lower swirling conical cavity. The longitudinal section of the guide fluid 26 is spindle-shaped. The ratio of the vertical distance between the tubular distributor 4 and the gas distribution plate 7 to the height of the reaction chamber 2 is 0.03.

[0082] The reactants in the fluidized bed reactor were m-xylene, ammonia, and air in a molar ratio of 1:5.8:23.4. The reaction temperature was 415℃, the pressure was 0.05MPa, the apparent linear velocity of the gas was 0.4m / s, the non-uniformity was 0.033, and the yield of isophthalonitrile was 83.1%.

[0083] Example 2

[0084] The branch pipe 13 of the tubular distributor 4 is composed of three connected circular pipes of different diameters. Along the flow direction within the pipe, the diameter ratio of the three circular pipes is 1:0.75:0.25, and correspondingly, the ratio of the three pipes to the total length of the branch pipe 13 is 0.7:0.15:0.15. The branch pipe 14 is connected to the branch pipe 13 via a flow-rectifying component 16. The angle α between the outer contour of the straight pipe shell 17 and the main flow direction 15 of the branch pipe 13 is 135°. The outer contour of the flow-rectifying component, a curved surface with varying diameters, is an elliptical arc. The internal flow channel of the flow component has an elliptical cross-section; swirling nozzles are evenly spaced on the branch pipe 14, wherein the nozzle inlet 21 extends along the spiral direction of the inner circumferential wall of the shell, has a square cross-section, and an included angle β of 120°. The height and diameter of the cylindrical upper swirling cavity of the nozzle are the same, and the top diameter of the lower swirling conical cavity is the same as the bottom diameter of the upper swirling cavity, with a bottom diameter to top diameter ratio of 0.25; the central column of the swirling nozzle is a conical column, with a large end diameter to small end diameter ratio of 1.25. The connection surface between the central column of the swirling nozzle and the guide fluid is 0.05 times the bottom diameter of the central column above the lower end face of the lower swirling conical cavity. The longitudinal cross-section of the guide fluid 26 is spindle-shaped; the ratio of the vertical distance between the tubular distributor 4 and the gas distribution plate 7 to the height of the reaction chamber 2 is 0.06.

[0085] The reactants in the fluidized bed reactor were m-xylene, ammonia, and air in a molar ratio of 1:5.5:22.1. The reaction temperature was 415℃, the pressure was 0.05MPa, the apparent linear velocity of the gas was 0.4m / s, the non-uniformity was 0.04, and the yield of isophthalonitrile was 82.8%.

[0086] Example 3

[0087] The branch pipe 13 of the tubular distributor 4 is composed of three interconnected circular pipes of different diameters. Along the flow direction within the pipe, the diameter ratio of the three circular pipes is 1:0.75:0.35, and the corresponding proportions of the three pipes to the total length of the branch pipe 13 are 0.8:0.1:0.1. The branch pipe 14 is connected to the branch pipe 13 via a flow rectifying component 16. The angle α between the outer contour of the straight pipe shell 17 and the main flow direction 15 of the branch pipe 13 is 120°. The outer contour of the flow rectifying component's curved pipe shell is an arc. The internal flow channel cross-section of the flow rectifying component is elliptical, and swirling nozzles 19 are evenly spaced on the branch pipe 14. The nozzle inlet cross-section is square and extends along the tangent direction of the inner circumferential wall of the shell. The upper swirling cavity of the cylindrical nozzle has the same height and diameter, and the top diameter of the lower swirling conical cavity is the same as the bottom diameter of the upper swirling cavity. The ratio of the bottom diameter to the top diameter is 0.25. The central column of the swirling nozzle is a cylinder of equal diameter. The connection surface between the central column of the swirling nozzle and the guide fluid is flush with the lower end face of the lower swirling conical cavity. The longitudinal section of the guide fluid 26 is spindle-shaped. The ratio of the vertical distance between the tubular distributor 4 and the gas distribution plate 7 to the height of the reaction chamber 2 is 0.09.

[0088] The reactants in the fluidized bed reactor were toluene, ammonia, and air in a molar ratio of 1:3.5:12.5. The reaction temperature was 405℃, the pressure was 0.1MPa, the apparent linear velocity of the gas was 0.5m / s, the non-uniformity was 0.03, and the yield of benzonitrile was 84.5%.

[0089] Example 4

[0090] Unlike Example 1, the branch pipe 13 of the tubular distributor 4 is composed of two connected circular pipes of different diameters. Along the flow direction within the pipe, the diameter ratio between the two circular pipes is 1:0.45; simultaneously, the ratio of the two pipes to the total length of the branch pipe is 0.7:0.3. The connection surface between the central column 24 of the swirling nozzle and the guide fluid 26 is 0.05 times the diameter of the bottom end of the central column below the lower end face of the lower swirling conical cavity. The included angle β is 130°.

[0091] The reactants in the fluidized bed reactor were m-xylene, ammonia, and air in a molar ratio of 1:7:25.4. The reaction temperature was 415℃, the pressure was 0.05MPa, the apparent linear velocity of the gas was 0.4m / s, the non-uniformity was 0.05, and the yield of isophthalonitrile was 81.6%.

[0092] Example 5

[0093] Unlike Example 1, the branch pipe 14 of the tubular distributor 4 is a round pipe that is directly connected to the branch pipe 13 without being connected through the rectifier 16, but is directly perpendicular to each other; the non-uniformity is 0.062, and the isophthalonitrile yield is 79.5%.

[0094] Example 6

[0095] Unlike Example 1, the branch pipe 13 of the tubular distributor 4 is a circular pipe of equal diameter; the non-uniformity is 0.073, and the isophthalonitrile yield is 78.4%.

[0096] Comparative Example 1

[0097] Unlike Example 1, the tubular distributor 4 does not use the nozzle of the present invention but uses a standard tubular insertion nozzle in the prior art; the reaction temperature is 445°C, the non-uniformity is 0.088, and the isophthalonitrile yield is 78.0%.

[0098] Comparative Example 2

[0099] Unlike Example 1, as follows: Figure 10 As shown, a tubular distributor using existing technology is used, wherein the branch pipes and sub-branch pipes are both round pipes and are connected perpendicularly to each other, and standard tubular insert nozzles are arranged at equal intervals on the sub-branch pipes.

[0100] The reactants in the fluidized bed reactor were m-xylene, ammonia, and air in a molar ratio of 1:7:26.5. The reaction temperature was 455℃, the non-uniformity was 0.11, and the yield of isophthalonitrile was 75.8%.

[0101] Comparative Example 3

[0102] Unlike Example 3, as follows: Figure 10 As shown, a tubular distributor using existing technology is used, wherein the branch pipes and sub-branch pipes are both circular pipes and are connected perpendicularly to each other, and standard tubular insert nozzles are arranged at equal intervals on the sub-branch pipes.

[0103] The reactants in the fluidized bed reactor were toluene, ammonia, and air in a molar ratio of 1:4:16.5. The reaction temperature was 415℃, the non-uniformity was 0.094, and the benzonitrile yield was 78.1%.

[0104] The preferred embodiments of the present invention have been described in detail above with reference to the accompanying drawings; however, the present invention is not limited thereto. Within the scope of the inventive concept, various simple modifications can be made to the technical solutions of the present invention, including combinations of various specific technical features in any suitable manner. To avoid unnecessary repetition, the present invention will not describe the various possible combinations separately. However, these simple modifications and combinations should also be considered as the content disclosed in the present invention and are all within the protection scope of the present invention.

Claims

1. A swirl nozzle characterized by, The cyclone nozzle (19) comprises: a shell, which is formed with a cyclone cavity, the cyclone cavity comprising an upper cyclone cavity (22) and a lower cyclone cavity (23), a bottom end of the lower cyclone cavity (23) being formed with a bottom end opening, the shell being provided with a nozzle feed port (21) communicating with the upper cyclone cavity (22); a central column (24) arranged in the cyclone cavity, a bottom end of the central column (24) extending to the bottom end opening of the lower cyclone cavity (23), the bottom end of the central column (24) being connected with a flow guide body (26), a nozzle discharge port (25) in the form of an annular gap being formed between the flow guide body (26), the bottom end of the central column (24) and the bottom end opening of the lower cyclone cavity (23); wherein the material entering from the nozzle feed port (21) can flow along the inner peripheral wall of the cyclone cavity to form a downward cyclone around the central column (24), and the downward cyclone is umbrella-shaped sprayed through the nozzle discharge port (25).

2. The rotational flow nozzle of claim 1, wherein, The flow guide body (26) comprises a gradually expanding section with an axially downward cross section gradually increasing, and a small end of the gradually expanding section is connected to the bottom end of the central column (24).

3. The rotational flow nozzle of claim 2, wherein, The gradually expanding section is provided in the shape of a circular truncated cone, and a connecting surface of the gradually expanding section is located above, below or flush with a bottom end surface of the lower cyclone cavity (23), and a distance between the connecting surface and the bottom end surface of the lower cyclone cavity (23) in the height direction is 0-0.1 times of a diameter of the bottom end of the central column (24).

4. The rotational flow nozzle of claim 3, wherein, A gradually tapering section with an axially downward cross section gradually decreasing is arranged below the gradually expanding section, and the gradually tapering section is provided in the shape of a circular cone.

5. The rotational flow nozzle of claim 4, wherein, A buffer section is arranged between the gradually tapering section and the gradually expanding section.

6. The rotational flow nozzle of claim 5, wherein, The buffer section is in the shape of a cylinder or a drum with a middle bulge.

7. The rotational flow nozzle of claim 1, wherein, The nozzle feed port (21) is connected to a peripheral wall of the shell and communicates with the upper cyclone cavity (22), and the nozzle feed port (21) extends in the tangential direction, the involute direction or the spiral direction of the inner peripheral wall of the shell; and / or An included angle between a line connecting an intersection point of a first inner wall (211) of the nozzle inlet (21) and an inner peripheral wall of the housing and a tangent line of the intersection point and a center of the housing β is 60°~120°; and / or A normal section of a material flow direction of the nozzle feed port (21) is one of a rectangle, a circle or an ellipse; and / or The upper cyclone cavity (22) is a cylindrical or circular truncated cone cavity; and / or The lower cyclone cavity (23) is arranged in the shape of a downward tapering conical cavity, a bottom end of the conical cavity is formed with the bottom end opening, a top end diameter of the conical cavity is the same as a diameter of the bottom end of the upper cyclone cavity (22), and a ratio of a bottom end diameter of the conical cavity to the top end diameter is 0.1-10.

8. The rotational flow nozzle of claim 7, wherein, A ratio of a height of the cylindrical cavity and / or the circular truncated cone cavity to a diameter of a middle position circle is 0.1-10.

9. The rotational flow nozzle of claim 8, wherein, A ratio of a maximum diameter to a minimum diameter of the circular truncated cone cavity is 0.1-10.

10. A tubular distributor characterized by The tubular distributor (4) comprises a branch pipe (13) and a plurality of branch pipes (14) communicating with the branch pipe (13), a plurality of cyclone nozzles (19) according to any one of claims 1-9 are installed on the branch pipes (14), and a connection end of the branch pipes (14) with the branch pipe (13) is provided with a flow straightening member (16) capable of strengthening flow distribution.

11. The tubular distributor of claim 10, wherein, The pipe distributor (4) is a branched pipe distribution structure; a plurality of branch pipes (14) are arranged on both sides of the branch pipe (13); and / or The cross section of the branch pipe (14) is circular, oval or rectangular.

12. The tubular distributor of claim 11, wherein, The branch pipe (14) extends along the radial direction of the branch pipe (13), one end of the branch pipe (14) is connected to the side of the branch pipe (13) through a flow regulating member (16), and the other end is closed.

13. The tubular distributor of claim 12, wherein, Along the main flow direction (15) of the material, the branch pipe (13) is a tapered pipe with a gradually decreasing cross section. and / or The ratio of the maximum diameter to the minimum diameter of the branch pipe (13) is 0.1-0.

9.

14. The tubular distributor of claim 13, wherein, The branch pipe (13) is a circular pipe, and the ratio of the large end diameter to the small end diameter of the circular pipe is 0.1-0.

9.

15. The tubular distributor of claim 14, wherein, The branch pipe (13) is composed of a plurality of circular pipes with different diameters connected end to end.

16. The tubular distributor of claim 15, wherein, The length of each section of the circular pipe accounts for 0.05-0.95 of the total length of the branch pipe (13).

17. The tubular distributor of claim 16, wherein, The pipe distributor (4) further comprises a main pipe (12), a plurality of branch pipes (13) are arranged on the side of the main pipe (12), and one end of the branch pipe (13) is connected to the main pipe (12) and the other end is closed.

18. The tubular distributor of claim 10 wherein, The flow regulating member (16) is a section of variable diameter pipe, the large end of the flow regulating member (16) is connected to the radial direction of the branch pipe (13), and the small end is connected to the branch pipe (14). and / or Along the flow direction in the flow regulating member (16), the profile of the variable diameter curved pipe shell (18) is one of circular arc, elliptical arc or parabolic.

19. The tubular distributor of claim 18, wherein, The pipe shell surrounding the flow regulating member (16) is composed of a straight pipe shell (17) and a variable diameter curved pipe shell (18).

20. The tubular distributor of claim 19, wherein, The angle α between the outer contour of the straight pipe shell (17) and the main flow direction (15) of the branch pipe (13) is 90-175°.

21. A fluidized bed reactor apparatus characterized by, The fluidized bed reaction device has a reaction chamber (2), and a material distributor is arranged in the reaction chamber (2), wherein the material distributor comprises the pipe distributor (4) according to any one of claims 10-20.

22. The fluidized bed reaction apparatus according to claim 21, wherein, The material distributor comprises at least one pipe distributor (4) and a gas distribution plate (7).

23. The fluidized bed reaction apparatus according to claim 21, wherein, The ratio of the vertical distance between the gas distribution plate (7) and the adjacent pipe distributor (4) to the height of the reaction chamber (2) is 0.01-0.

1.

24. The use of the cyclone nozzle according to any one of claims 1-9 or the pipe distributor according to any one of claims 10-20 or the fluidized bed reaction device according to any one of claims 21-23 in hydrocarbon ammoxidation, catalytic cracking, nitrobenzene hydrogenation or coal gasification reaction.

25. A method of hydrocarbon ammoxidation reaction, characterized by, The method uses the fluidized bed reaction device according to any one of claims 21-23, and the material distributor comprises at least one pipe distributor (4) and a gas distribution plate (7).

26. The method of claim 25, wherein, The method comprises: The raw material containing hydrocarbon source and ammonia source enters the reaction chamber (2) through the pipe distributor (4), and the oxygen-containing gas enters the reaction chamber (2) through the gas distribution plate (7); The raw material containing a hydrocarbon source and an ammonia source is reacted with an oxygen-containing gas in the reaction cavity.

27. The method of claim 26, wherein, The raw material containing a hydrocarbon source and an ammonia source is reacted with an oxygen-containing gas in the reaction cavity.

28. The method of claim 26, wherein, The non-uniformity of the discharge flow of the tubular distributor (4) is 0-0.35; and / or The molar ratio of the hydrocarbon source, the ammonia source and the oxygen-containing gas is 1:(1-10):(10-40) in terms of hydrocarbon groups, amino groups and oxygen molecules respectively; And / or The ammonia source is ammonia gas; And / or The contact conditions include: a reaction temperature of 300-500 ℃, a pressure of 0.01-0.2 MPa, and a gas apparent linear velocity of 0.1-0.8 m / s.

29. The method of claim 28, wherein, The hydrocarbon source includes hydrocarbons and / or hydrocarbon derivatives.

30. The method of claim 29, wherein, The hydrocarbon source includes at least one of toluene, p-chlorotoluene, o-chlorotoluene, o-xylene, m-xylene, p-xylene, dichlorotoluene, trichlorotoluene and 4-nitro-o-xylene.

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