Spiral-flow type nozzle, tubular distributor, fluidized bed reaction device and hydrocarbon ammoxidation reaction method

Abstract

The invention relates to the technical field of chemical equipment, and discloses a spiral-flow type nozzle, a tubular distributor, a fluidized bed reaction device and a hydrocarbon ammoxidation reaction method. The spiral-flow type nozzle comprises a shell, a spiral-flow cavity is defined by the shell and comprises an upper spiral-flow cavity body and a lower spiral-flow cavity body, a bottom end opening is formed in the bottom end of the lower spiral-flow cavity body, and the shell is provided with a nozzle feeding port communicated with the upper spiral-flow cavity body; and the central column is arranged in the rotational flow cavity, the bottom end of the central column extends towards the opening in the bottom end of the lower rotational flow cavity, the bottom end of the central column is connected with a flow guide body, and a nozzle discharge port with an annular gap is formed among the flow guide body, the bottom end of the central column and the opening in the bottom end of the lower rotational flow cavity. The uniform gas distribution performance of the tubular distributor can be enhanced, and furthermore, the yield of ammoxidation products can be improved.

Description

Technical Field

[0001] The invention relates to the technical field of chemical equipment, and in particular to a swirl nozzle, a tubular distributor, a fluidized bed reaction device and a method for hydrocarbon ammoxidation reaction. Background Art

[0002] Tubular distributor is a kind of gas distributor commonly used in catalytic cracking and hydrocarbon ammoxidation reactors. It is characterized by a free end, which can solve the problems of thermal expansion and multi-stage gas feeding. It is especially suitable for large reactors and processes that require multiple groups of gas feeds. At present, the tubular distributor is composed of a main pipe, a branch pipe, a branch pipe and a nozzle.

[0003] CN204017797U discloses a feed distributor for an ammonia oxidation reactor. The various sections of the distributor are attached to each other and the wall of the reactor using gas-tight quick disconnect fittings to facilitate the replacement of different sections of the feed distributor used in a commercial ammonia oxidation reactor. In addition, the diameter of the branch pipes in these distributor sections and the diameter of the feed nozzles attached to these branch pipes are changed to facilitate the uniform flow of the feed gas through these components. The distributor can be subdivided into a plurality of feed distributor sections arranged for better reactor control. Finally, the end cap terminated at the far end of the distributor branch pipe can be provided with a nozzle for removing any ammonia oxidation catalyst that may accidentally reach the inside of the distributor. However, as the size of the reactor is enlarged, the problem of uneven flow field in the distributor is further exacerbated. Summary of the invention

[0004] Most of the existing tubular distributor nozzles are simply short tubes connected to branch pipes. When the airflow enters the nozzle from the branch pipe, the sudden change in flow direction may cause serious deviation, or even cause the backflow of materials (such as catalysts) outside the tubular distributor due to local decompression. Although a type of pressure swirl nozzle commonly used in liquid atomization has good uniform distribution performance, it is difficult to apply to reactors containing particulate materials (such as catalyst particles) due to the strong back suction effect caused by central centrifugal decompression. Furthermore, it is also difficult to apply to hydrocarbon ammoxidation reactions that use more tubular distributors. Based on the foregoing, the purpose of the present invention is to overcome the problems existing in the prior art, and through a large amount of CFD simulation and flow field analysis and specific experimental research, a swirl nozzle, a tubular distributor, a fluidized bed reaction device and a method for hydrocarbon ammoxidation reaction are provided, which can enhance the uniform gas distribution performance of the tubular distributor, and further have the effect of improving the yield of the ammoxidation product.

[0005] In order to achieve the above object, the present invention provides a swirl nozzle on one hand, the swirl nozzle comprising:

[0006] A shell, wherein the shell is surrounded by a swirl chamber, the swirl chamber includes an upper swirl chamber and a lower swirl chamber, the bottom end of the lower swirl chamber is formed with a bottom opening, and the shell is provided with a nozzle feed port connected to the upper swirl chamber;

[0007] A center column is arranged in the cyclone chamber, the top end of the center column is connected to the shell top wall of the cyclone chamber, the bottom end of the center column extends to the bottom opening of the lower cyclone chamber, the bottom end of the center column is connected to a guide body, and a nozzle discharge port with an annular gap is formed between the guide body, the bottom end of the center column and the bottom opening of the lower cyclone chamber;

[0008] The material entering from the nozzle feed port can flow on the inner peripheral wall of the swirl chamber to form a downward swirl around the central column, and the downward swirl is ejected in an umbrella shape through the nozzle discharge port.

[0009] The second aspect of the present invention provides a tubular distributor, which includes a branch pipe and a plurality of branch pipes connected to the branch pipe, a plurality of swirl nozzles according to the present invention are installed on the branch pipe, and the connecting ends of the branch pipe and the branch pipe are provided with rectifying components capable of enhancing logistics distribution.

[0010] A third aspect of the present invention provides a fluidized bed reaction device, which comprises a reaction chamber, wherein a material distributor is arranged in the reaction chamber, and the material distributor comprises the tubular distributor described in the present invention.

[0011] A fourth aspect of the present invention provides the use of the swirl nozzle of the present invention, the tubular distributor of the present invention, or the fluidized bed reaction device of the present invention in ammonia oxidation, catalytic cracking, nitrobenzene hydrogenation or coal gasification reaction.

[0012] The fifth aspect of the present invention provides a method for hydrocarbon ammoxidation reaction, which adopts the fluidized bed reaction device of the present invention, and the material distributor includes at least one tubular distributor and a gas distribution plate;

[0013] Preferably, the method comprises:

[0014] The raw materials containing hydrocarbon source and ammonia source enter the reaction chamber through the tubular distributor.

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

[0016] In the reaction chamber, the raw material containing hydrocarbon source and ammonia source is contacted with oxygen-containing gas for reaction. Preferably, the raw material containing hydrocarbon source and ammonia source is contacted with oxygen-containing gas for reaction in reverse direction.

[0017] Through the above technical scheme, the swirl nozzle of the present invention allows the incoming material to flow on the inner wall of the swirl chamber to form a downward swirl around the central column, and is ejected in an umbrella shape through the nozzle discharge port. 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 the backflow of materials outside the swirl nozzle caused by local decompression; the rectifying component of the tubular distributor of the present invention can eliminate the gas deviation inside the tubular distributor, so that the gas distribution performance of the distributor is closer to the ideal gas distribution state, and the uniform distribution of the gas flow is enhanced; further, the reaction materials of the fluidized bed reaction device of the present invention are closer to the ideal gas distribution state, so that the reaction materials are fully contacted and the raw material conversion rate is improved; further, the method of hydrocarbon ammoxidation reaction of the present invention has the effect of improving the yield of ammoxidation products and reducing the amount of raw materials. BRIEF DESCRIPTION OF THE DRAWINGS

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

[0019] Figure 2 yes Figure 1 Schematic diagram of the structure of the middle tube distributor;

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

[0021] Figure 4 yes Figure 2 A schematic diagram of a branch pipe-branch pipe in one form;

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

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

[0024] Figure 7 yes Figure 2 Schematic diagram of the three-dimensional structure of the medium swirl nozzle;

[0025] Figure 8 It is a structural schematic diagram of a longitudinal section of a swirl nozzle;

[0026] Fig. 9 It is a schematic diagram of the cross-sectional structure of the swirl nozzle at the nozzle feed inlet;

[0027] Fig.10 It is a structural schematic diagram of a tubular distributor in the prior art;

[0028] Fig.11This is a flow distribution comparison diagram of the distributor using the variable diameter and rectifying components of the present invention and the conventional distributor.

[0029] Description of Reference Numerals

[0030] 1 is a gas collecting chamber; 2 is a reaction chamber; 3 is a heat exchange device; 4 is a tubular distributor; 5 is a hydrocarbon source; 6 is an ammonia source; 7 is a gas distribution plate; 8 is an oxygen-containing gas; 9 is a second material inlet; 10 is a cyclone separator; 11 is a first material outlet; 12 is a main pipe; 13 is a branch pipe; 14 is a branch pipe; 15 is the mainstream direction of the logistics; 16 is a rectifying component; 17 is a straight tube shell; 18 is a different-diameter curved tube shell; 19 is a swirl nozzle; 20 is the incoming gas in the branch pipe; 21 is a nozzle feed port; 22 is an upper swirl chamber; 23 is a lower swirl chamber; 24 is a central column; 25 is a nozzle discharge port; 26 is a guide body; 211 is a first inner wall. DETAILED DESCRIPTION

[0031] The specific implementation of the present invention is described in detail below in conjunction with the accompanying drawings. It should be understood that the specific implementation described here is only used to illustrate and explain the present invention, and is not used to limit the present invention.

[0032] The endpoints and any values ​​of the ranges disclosed in this article 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 each range, the endpoint values ​​of each range and the individual point values, and the individual point values ​​can be combined with each other to obtain one or more new numerical ranges, which should be considered as specifically disclosed in this article.

[0033] In the present invention, unless otherwise specified, directional words such as "up, down, top, bottom" are usually used with reference to the directions shown in the drawings or are used to describe the relative positional relationships of components in the vertical, perpendicular or gravity directions; "inside and outside" usually refer to the inside and outside of a chamber relative to an inner chamber or the radial inside and outside relative to the center of a circle.

[0034] like Figure 7-Figure 8 As shown, the first aspect of the present invention provides a swirl nozzle, the swirl nozzle 19 comprises:

[0035] A shell, wherein a swirl chamber is formed around the shell, and the swirl chamber includes an upper swirl chamber 22 and a lower swirl chamber 23, wherein the lower swirl chamber 23 is configured as a tapered chamber that tapers downward, and a bottom opening is formed at the bottom end of the tapered chamber, and the shell is provided with a nozzle feed port 21 connected to the upper swirl chamber 22;

[0036] The center column 24 is arranged in the swirl chamber, the top of the center column 24 is connected to the top wall of the shell of the swirl chamber, the bottom of the center column 24 extends to the bottom opening of the lower swirl chamber 23, the bottom of the center column 24 is connected to the guide body 26, and the nozzle outlet 25 with an annular gap is formed between the guide body 26, the bottom end of the center column 24 and the bottom opening of the lower swirl chamber 23. Figure 8 As shown, the entire shell is sleeved around the center column 24 and the guide body 26 , but does not contact the guide body 26 .

[0037] Among them, the material entering from the nozzle feed port 21 can flow on the inner wall of the swirl chamber to form a downward swirl around the central column 24, and the downward swirl is ejected in an umbrella shape through the nozzle discharge port 25. In this way, on the one hand, a more optimized material flow distribution effect can be achieved; on the other hand, the influence of backflow of materials (such as catalysts) outside the swirl nozzle caused by local decompression can be eliminated.

[0038] like Figure 8 As shown, according to a preferred embodiment of the present invention, the flow guide 26 includes a gradually expanding section whose cross section gradually increases in the axial downward direction, the small end of the gradually expanding section is connected to the bottom end of the center column 24, and the cross-sectional area of ​​the large end of the gradually expanding section is larger than the area of ​​the bottom end opening of the lower swirl chamber 23;

[0039] It should be noted that, in the present invention, the material that is backflowed into the swirl nozzle 19 is taken as an example of catalyst particles, but the present invention is not limited to this. In some embodiments, in the fluidized bed reaction device, the catalyst particles will be carried upward by the gas (such as air) of the bottom feed, and the nozzle outlet 25 of the swirl nozzle 19 is located above the gas feed port of the bottom feed, and the nozzle outlet 25 is facing the bottom of the fluidized bed reaction device. In this way, since the gas velocity of the nozzle outlet 25 is greater, the formation of local decompression will cause the catalyst particles that are upward with the gas to be sucked into the swirl nozzle, and the gradually expanding section of the guide body 26 can prevent the backflow of the catalyst; further, the gradually expanding section is set to be a truncated cone, and the small end of the truncated cone is connected to the bottom end of the center column 24, and the connection surface of the two can be located above, below or flush with the bottom end surface of the conical cavity; the distance between the connection surface of the gradually expanding section and the center column 24 and the bottom end surface of the conical cavity in the height direction is 0 to 0.1 times the diameter of the center column 24.

[0040] In the present invention, the central column 24 can be a cylindrical column with a constant diameter or a tapered column with a diameter gradually decreasing from top to bottom, and the ratio of the large end diameter to the small end diameter of the tapered column is 1 to 1.5.

[0041] According to a preferred embodiment of the present invention, a tapered section with a gradually decreasing cross-section axially downward is provided below the gradually expanding section; the tapered section is configured to be conical, so that when the gas carrying particulate matter, such as catalyst particles, fed from below the swirl nozzle 19 passes through the conical tapered section upward, the catalyst particles are dispersed, which increases the contact area with the reaction materials on the one hand, and on the other hand, the dispersed catalyst is also away from the nozzle outlet 25, thereby avoiding being sucked into the nozzle due to the pressure difference.

[0042] According to a preferred embodiment of the present invention, the tapering section and the gradually expanding section are connected by a buffer section. The tapering section, the buffer section and the gradually expanding section can be integrally formed, and the buffer section is cylindrical or drum-shaped with a raised middle portion, so that the longitudinal cross-section of the flow guide 26 is roughly elliptical or spindle-shaped; wherein the buffer section located in the middle increases the spacing between the tapering section and the gradually expanding section, so that the particles dispersed through the conical tapering section can be further away from the nozzle outlet 25 when reaching the height of the nozzle outlet 25 to avoid being sucked into the nozzle 19, thereby eliminating the influence of backflow.

[0043] In the present invention, the nozzle feed port 21 is connected to the peripheral wall of the shell and communicates with the upper swirl chamber 22. The nozzle feed port 21 extends along the tangent direction, involute direction or spiral direction of the inner peripheral wall of the shell, so that the material is fed along the tangent direction, involute direction or spiral direction of the swirl chamber 22; Figure 7 As shown, in some embodiments of the present invention, the nozzle feed port 21 extends along the tangent direction of the inner circumferential wall of the shell.

[0044] In the present invention, Fig. 9 As shown, the angle β between the intersection of the first inner wall 211 of the nozzle feed port 21 and the inner circumferential wall of the shell and the line connecting the center of the shell and the tangent of the intersection is 60° to 120°.

[0045] In the present invention, the normal cross section of the nozzle feed port 21 in the material flow direction is one of rectangular, circular or elliptical.

[0046] In the present invention, the upper swirl chamber 22 is a cylindrical or truncated cone-shaped chamber.

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

[0048] In the present invention, the ratio of the maximum diameter to the minimum diameter of the truncated cone-shaped cavity is more preferably 0.1-10.

[0049] In the present invention, the top diameter of the conical cavity is the same as the bottom diameter of the upper swirl 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 swirl cavity of the nozzle in the present invention is not limited to Figure 7-Figure 8The downwardly tapering conical cavity shown in the figure may also be a downwardly expanding conical cavity according to actual use requirements. In the embodiments of the present invention, only the downwardly tapering conical cavity is used as an example to illustrate the advantages of the present invention, but the present invention is not limited to this.

[0050] like Figure 4-Figure 6 As shown, the second aspect of the present invention provides a tubular distributor 4, including a branch pipe 13 and a plurality of branch pipes 14 connected to the branch pipe 13, a plurality of swirl nozzles 19 of the present invention are installed on the branch pipe 14, and a rectifying component 16 is provided at the connecting end of the branch pipe 14 and the branch pipe 13, so that the gas bias flow inside the tubular distributor 4 can be eliminated, thereby strengthening the uniform distribution of the gas flow rate, such as Fig.11 As shown, CFD analysis shows that the above components can significantly suppress the deviation flow and turbulence in the distributor and enhance the uniform distribution of flow.

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

[0052] In the present invention, the branch pipe 14 is extended 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 rectifying component 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 mainstream direction 15 of the logistics, the branch pipe 13 is a tapered pipe with a gradually decreasing cross-section of the tube cavity; in this way, the gas flow rate from the branch pipe 13 to the branch pipe 14 can be evenly distributed. Furthermore, the branch pipe 13 is preferably a round pipe, and the ratio of the large end diameter to the small end diameter of the round pipe is 0.1 to 0.9; more preferably, the branch pipe 13 is composed of multiple sections of round pipes with different diameters connected end to end; further preferably, the length of each section of the round pipe accounts for 0.05 to 0.95 of the total length of the branch pipe 13; further, 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 the present invention, the tubular distributor 4 also includes a main pipe 12, and a plurality of branch pipes 13 are provided, and the plurality of branch pipes 13 are radially 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 set to be closed.

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

[0055] According to a preferred embodiment of the present invention, the rectifying member 16 is a pipe with a variable diameter, such as Figure 4-Figure 6 As shown, the large end of the 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 rectifying member 16 and the branch pipe have various shapes, such as Figure 4 or Figure 5 As shown, the flow cross-section of the rectifying component 16 is circular, elliptical or rectangular to connect with the corresponding circular or square branch pipes. In the embodiment of the present invention, the circular branch pipe is used as an example to illustrate the advantages of the present invention, but the present invention is not limited to this.

[0056] According to a preferred embodiment of the present invention, the tube shell surrounding the rectifying member 16 can be regarded as consisting of a straight tube shell 17 and a different-diameter curved tube shell 18 in the axial direction, that is, the straight tube shell 17 and the different-diameter curved tube shell 18 located below the straight tube shell 17 together form a variable-diameter tube cavity of the rectifying member 16, wherein the radial cross-section of the different-diameter curved tube shell 18 is an inward-concave arc with the center at the top, and the diameter of the inward-concave arc gradually decreases along the logistics direction inside the rectifying member 16 until the cross-sectional area of ​​the tube cavity formed by the straight tube shell 17 is the same as the cross-sectional area of ​​the branch pipe 14; specifically, viewed from the longitudinal cross-sectional direction of the rectifying member 16, along the logistics direction inside the rectifying member 16, the profile of the different-diameter curved tube shell 18 is one of a circular arc, an elliptical arc or a parabola; the straight tube shell 17 and the different-diameter curved tube shell 18 are smoothly transitionally connected in the radial direction to reduce the resistance of the airflow flowing through the inside of 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 mainstream direction 15 of the branch pipe 13 is 90° to 175°; along the logistics direction in the rectifying component 16, the profile of the different-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 reaction device, which comprises a reaction chamber 2, in which a material distributor is arranged, and the material distributor comprises the tubular distributor 4 of the present invention.

[0059] In the present 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 reaction device of the present invention is used in the ammonia oxidation reaction, and also includes some structures of the conventional ammonia oxidation reaction device in the prior art, such as a gas collecting chamber, a cyclone separator and a heat exchange device, etc. Specifically, for example, in some embodiments of the present invention, Figure 1As shown, the fluidized bed reaction device has a reaction chamber 2 and is provided 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 provided in the reaction chamber 2, and the first material inlet is connected to the tubular distributor 4 of the present invention; specifically, the first material outlet 11 is arranged at the top of the fluidized bed reaction device, and the second material outlet equipped with a control valve is arranged at the bottom of the fluidized bed reaction device. A necking section is formed at the lower part of the reaction chamber, and the bottom end of the necking section extends downward to form a second material outlet; the first material outlet 11 is connected to the gas collecting chamber 1; the gas collecting chamber 1 is connected to the cyclone separator 10, and the product gas after the reaction passes through the cyclone separator 10 to separate the catalyst particles and then enters the gas collecting chamber 1 and is discharged from the first material outlet; in the present invention, the first material The inlet is arranged 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 swirl 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 arranged below the first material inlet, and the second material inlet is arranged as a pipeline radially penetrating the cavity wall of the necking section, and the pipeline located in the reaction chamber is bent downward, so that the gas entering through the second material inlet 9 is reflected by the cavity wall of the necking section, dispersed upward, and distributed upward again through the gas distribution plate 7 arranged above the second material inlet 9; the gas distribution plate 7 is arranged below the tubular distributor 4; in this way, the material of the first material inlet is in countercurrent contact with the material of the second material inlet, and is fully reacted.

[0061] The fourth aspect of the present invention provides the use of the swirl nozzle of the present invention, the tubular distributor of the present invention, or the fluidized bed reaction device of the present invention in hydrocarbon ammoxidation, catalytic cracking, nitrobenzene hydrogenation or coal gasification reaction.

[0062] A fifth aspect of the present invention provides a method for ammoxidation of hydrocarbons. The method is carried out in a fluidized bed reaction device of the present invention. The material distributor includes at least one tubular distributor 4 and a gas distribution plate 7.

[0063] In the present invention, preferably, the method comprises: a raw material containing a hydrocarbon source and an ammonia source enters the reaction chamber 2 through a tubular distributor 4, and an oxygen-containing gas enters the reaction chamber 2 through a gas distribution plate 7; in the reaction chamber, the raw material containing a hydrocarbon source and an ammonia source contacts and reacts with the oxygen-containing gas, preferably, the raw material containing a hydrocarbon source and an ammonia source contacts and reacts with the oxygen-containing gas in reverse.

[0064] After the raw materials containing hydrocarbon source and ammonia source are sprayed out from the tubular distributor 4 and the swirl nozzle 19 of the present invention, they are mixed with oxygen-containing gas and undergo ammonia oxidation reaction under the action of a catalyst, thereby improving the uniformity and utilization rate of the raw material distribution, thereby increasing the yield of the ammonia oxidation product.

[0065] In the present invention, the unevenness of the flow rate of the tubular distributor 4 can reach 0 to 0.35; wherein, the unevenness calculation method in the present invention is: Where n is the number of swirl nozzles 19, u i is the spray flow rate of the swirl nozzle 19, is the average flow rate sprayed by the swirl nozzle 19, for example, n can be 200-5000.

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

[0067] In the present invention, the catalyst is pre-loaded above the gas distribution plate 7, and the oxygen-containing gas entering from the second material inlet at the bottom carries the catalyst to contact and mix with the raw material containing the hydrocarbon source and the ammonia source, and a crude nitrile product gas is obtained after the reaction. The crude nitrile product gas enters the cyclone separator 10 to separate the catalyst and then enters the gas collecting chamber 1. The catalyst separated from the cyclone separator 10 falls back to the bed layer in the reaction zone from the material leg.

[0068] In the present invention, the molar ratio of the hydrocarbon source in terms of hydrocarbon groups, the ammonia source in terms of amino groups and the oxygen-containing gas in terms of oxygen molecules is preferably 1:(1-10):(10-40).

[0069] In the present invention, the hydrocarbon source preferably 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 the present invention, the ammonia source is selected from ammonia or a mixed gas containing ammonia. In the present invention, the oxygen-containing gas is selected from oxygen or a mixed gas containing oxygen, such as air. The present invention has no special requirements for the ammonia source and the oxygen-containing gas, which will not be elaborated here.

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

[0072] The catalyst in the present invention is a catalyst commonly used in the prior art for hydrocarbon ammoxidation reaction, for example, NC-III type or other vanadium-chromium series silica carrier particle catalyst.

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

[0074] In the embodiments of the present invention, the oxygen-containing gas is illustrated by air, the ammonia source is illustrated by ammonia, and the catalyst is illustrated by NC-III (the present invention has no special requirements for the catalyst, and the catalysts commonly used in the art can be applied to the present invention);

[0075] The following examples are Figure 1-Figure 8 The fluidized bed reaction device shown in the figure is carried out, and the fluidized bed reaction device has a reaction chamber 2, and a heat exchange device 3 and a tubular distributor 4 are arranged in the reaction chamber 2; a first material outlet 11 is arranged at the top of the reaction chamber, and the first material outlet 11 is connected to the gas collecting chamber 1, and the gas collecting chamber 1 is connected to the cyclone separator 10; a first material inlet connected to the tubular distributor 4 is arranged below the cyclone separator 10, and the nozzle outlet 25 of the cyclone nozzle 19 faces the bottom space of the reaction chamber 2; a second material inlet 9 is arranged below the first material inlet, and a gas distribution plate 7 is arranged below the tubular distributor 4;

[0076] The tubular distributor 4 includes a main pipe 12, and a plurality of branch pipes 13 are radially 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 set to be closed, and the branch pipe 13 is composed of multiple sections of circular pipes with different diameters connected end to end; a plurality of branch pipes 14 are extended 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 rectifying component 16, and the other end is set to be closed; the rectifying component 16 is a pipe with a variable diameter, the large end of the rectifying component 16 is connected to the radial direction of the branch pipe 13, and the small end is connected to the branch pipe 14; the tube shell surrounding the rectifying component 16 is composed of a straight tube shell 17 and a different diameter curved surface tube shell 18; the straight tube shell 17 and the different diameter curved surface tube shell 18 are smoothly transitioned and connected in the radial direction; along the flow direction in the rectifying component 16, the profile of the different diameter curved surface tube shell 18 is parabolic.

[0077] The swirl nozzle 19 includes: a shell, a swirl chamber is formed around the shell, the swirl chamber includes an upper swirl chamber 22 and a lower swirl chamber 23, the lower swirl chamber 23 is set as a tapered chamber that tapers downward, and the bottom end of the tapered chamber is formed with a bottom opening, and the upper swirl chamber 22 opens a nozzle feed port 21; a center column 24 is set in the swirl chamber, the top of the center column 24 is connected to the shell top wall of the swirl chamber, the bottom end of the center column 24 extends to the bottom opening of the lower swirl chamber 23, the bottom end of the center column 24 is connected to a guide body 26, and a nozzle discharge port 25 with an annular gap is formed between the guide body 26, the bottom end of the center column 24 and the bottom opening of the lower swirl chamber 23; the guide body 26 includes a truncated cone-shaped gradually expanding section, a cylindrical buffer section and an inverted conical tapered section from top to bottom, and the small end of the truncated cone-shaped gradually expanding section is connected to the bottom end of the center column 24.

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

[0079] In the following examples 1-6, the number of branch pipes 13 of the tubular distributor 4 is 4, the number of branch pipes 14 is 14 per branch pipe, and the inlet flow rate of the main pipe 12 is 60m 3 / h, the unevenness of the spray flow rate of the tubular distributor 4 in Examples 1-6 can all reach 0 to 0.35.

[0080] Example 1

[0081] The branch pipe 13 of the tubular distributor 4 is composed of three sections of circular pipes with different diameters connected together. Along the flow direction in the pipe, the diameter ratio of the three sections of circular pipes is 1:0.75:0.35, and the corresponding three sections of pipes account for the total length of the branch pipe 13 in the ratio of 0.8:0.1:0.1; the branch pipe 14 is connected to the branch pipe 13 through a rectifying component 16; 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 160°, the outer contour line of the rectifying component with a different diameter curved surface tube shell is an arc, and the internal flow channel cross-section of the rectifying component is elliptical; the branch pipe 14 is evenly spaced with swirl-type Nozzle, wherein the nozzle feed port 21 extends along the involute direction of the inner circumferential wall of the shell, has a square cross-section, an angle β of 60°, the height and diameter of the cylindrical upper swirl chamber of the nozzle are the same, the top diameter of the lower swirl conical chamber is the same as the bottom end of the upper swirl chamber, and the ratio of the bottom diameter to the top diameter is 0.25; the swirl nozzle center column 24 is a cylinder of equal diameter, the connection surface between the swirl nozzle center column and the guide body is flush with the lower end surface of the lower swirl conical chamber, and the longitudinal section of the guide body 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 reaction raw materials in the fluidized bed reactor are meta-xylene, ammonia and air, the molar ratio is 1:5.8:23.4, the reaction temperature is 415°C, the pressure is 0.05MPa, the gas superficial velocity is 0.4m / s, the heterogeneity is 0.033, and the yield of isophthalonitrile is 83.1%.

[0083] Example 2

[0084] The branch pipe 13 of the tubular distributor 4 is composed of three sections of circular pipes with different diameters connected together. Along the flow direction in the pipe, the diameter ratio of the three sections of circular pipes is 1:0.75:0.25, and the corresponding three sections of pipes account for the total length of the branch pipe 13 in a ratio of 0.7:0.15:0.15. The branch pipe 14 is connected to the branch pipe 13 through a 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 rectifying component with a different diameter curved surface is an elliptical arc. The cross section of the flow channel inside the flow component is elliptical; the branch pipe 14 is evenly spaced with swirl nozzles, wherein the nozzle feed port 21 extends along the spiral line direction of the inner peripheral wall of the shell, the cross section is square, the angle β is 120°, the height and diameter of the cylindrical upper swirl chamber of the nozzle are the same, the top diameter of the lower swirl conical chamber is the same as the bottom end of the upper swirl chamber, and the ratio of the bottom diameter to the top diameter is 0.25; the central column of the swirl nozzle is a conical column, and the ratio of the large end diameter of the central column to the small end diameter is 1.25. The connection surface between the central column of the swirl nozzle and the guide body is higher than the bottom end face of the lower swirl conical chamber by 0.05 times the diameter of the bottom end of the central column, and the longitudinal cross section of the guide body 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 reaction raw materials in the fluidized bed reactor are meta-xylene, ammonia and air, the molar ratio is 1:5.5:22.1, the reaction temperature is 415°C, the pressure is 0.05 MPa, the gas superficial velocity is 0.4 m / s, the unevenness is 0.04, and the yield of isophthalonitrile is 82.8%.

[0086] Example 3

[0087] The branch pipe 13 of the tubular distributor 4 is composed of three sections of circular pipes with different diameters. Along the flow direction in the pipe, the ratio of the diameters of the three sections of circular pipes is 1:0.75:0.35, and the corresponding three sections of pipes account for the total length of the branch pipe 13 in the ratio of 0.8:0.1:0.1. The branch pipe 14 is connected to the branch pipe 13 through a rectifying component 16. 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 120°. The outer contour of the rectifying component with a different diameter curved surface is an arc. The cross section of the internal flow channel of the rectifying component is elliptical, and swirl nozzles 19 are arranged at equal intervals on the branch pipe 14. The cross section of the nozzle feed port is square and extends along the tangent direction of the inner peripheral wall of the shell. The height and diameter of the cylindrical upper swirl chamber of the nozzle are the same, the top diameter of the lower swirl conical chamber is the same as the bottom of the upper swirl chamber, and the ratio of the bottom diameter to the top diameter is 0.25; the central column of the swirl nozzle is a cylinder of equal diameter, the connection surface between the central column of the swirl nozzle and the guide body is flush with the lower end surface of the lower swirl conical chamber, and the longitudinal section of the guide body 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 reaction raw materials in the fluidized bed reactor are toluene, ammonia and air, the molar ratio is 1:3.5:12.5, the reaction temperature is 405°C, the pressure is 0.1 MPa, the gas superficial velocity is 0.5 m / s, the heterogeneity is 0.03, and the yield of benzonitrile is 84.5%.

[0089] Example 4

[0090] The difference from Example 1 is that the branch pipe 13 of the tubular distributor 4 is composed of two sections of circular pipes with different diameters connected together. Along the flow direction in the pipe, the diameter ratio between the two sections of circular pipes is 1:0.45; at the same time, the ratio of the corresponding two sections of pipes to the total length of the branch pipe is 0.7:0.3. The connection surface between the central column 24 of the swirl nozzle and the guide body 26 is lower than the bottom end surface of the lower swirl conical cavity by 0.05 times the diameter of the bottom end of the central column. The angle β is 130°.

[0091] The reaction raw materials in the fluidized bed reactor are meta-xylene, ammonia and air, the molar ratio is 1:7:25.4, the reaction temperature is 415°C, the pressure is 0.05 MPa, the gas superficial velocity is 0.4 m / s, the unevenness is 0.05, and the yield of isophthalonitrile is 81.6%.

[0092] Example 5

[0093] The difference from Example 1 is that the branch pipe 14 of the tubular distributor 4 is a round pipe directly connected to the branch pipe 13 without being connected through the rectifying component 16 but directly connected to each other vertically; the unevenness is 0.062, and the yield of isophthalonitrile is 79.5%.

[0094] Example 6

[0095] The difference from Example 1 is that the branch pipe 13 of the tubular distributor 4 is a circular pipe with a constant diameter; the unevenness is 0.073, and the yield of isophthalonitrile is 78.4%.

[0096] Comparative Example 1

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

[0098] Comparative Example 2

[0099] The difference from Example 1 is that: Fig.10 As shown, a tubular distributor in the prior art is used, wherein the branch pipes and the branch pipes are all circular pipes and are vertically connected to each other, and standard tubular insert nozzles are arranged at equal intervals on the branch pipes.

[0100] The reaction raw materials in the fluidized bed reactor are m-xylene, ammonia and air, the molar ratio is 1:7:26.5, the reaction temperature is 455°C, the non-uniformity is 0.11, and the yield of isophthalonitrile is 75.8%.

[0101] Comparative Example 3

[0102] The difference from Example 3 is that: Fig.10 As shown, a tubular distributor in the prior art is used, wherein the branch pipes and the branch pipes are all circular pipes and are vertically connected to each other, and standard tubular insert nozzles are arranged at equal intervals on the branch pipes.

[0103] The reaction raw materials in the fluidized bed reactor are toluene, ammonia and air, the molar ratio is 1:4:16.5, the reaction temperature is 415°C, the non-uniformity is 0.094, and the yield of benzonitrile is 78.1%.

[0104] The preferred embodiments of the present invention are described in detail above in conjunction with the accompanying drawings, but the present invention is not limited thereto. Within the technical concept of the present invention, the technical solution of the present invention can be subjected to a variety of simple modifications, including the combination of various specific technical features in any appropriate manner. In order to avoid unnecessary repetition, the present invention will not further describe various possible combinations. However, these simple modifications and combinations should also be regarded as the contents disclosed by the present invention and belong to the protection scope of the present invention.

Claims

1. A swirl nozzle, characterized in that: The swirl nozzle (19) comprises: A shell, wherein the shell is surrounded by a swirl chamber, the swirl chamber comprises an upper swirl chamber (22) and a lower swirl chamber (23), a bottom end of the lower swirl chamber (23) is formed with a bottom end opening, and the shell is provided with a nozzle feed port (21) connected to the upper swirl chamber (22); A central column (24) is arranged in the swirl chamber, the bottom end of the central column (24) extends toward the bottom opening of the lower swirl chamber (23), the bottom end of the central column (24) is connected to a guide body (26), and a nozzle discharge port (25) with an annular gap is formed between the guide body (26), the bottom end of the central column (24) and the bottom opening of the lower swirl chamber (23); The material entering from the nozzle feed port (21) can flow on the inner peripheral wall of the cyclone chamber to form a downward cyclone around the central column (24), and the downward cyclone is ejected through the nozzle discharge port (25).

2. The swirl nozzle according to claim 1, characterized in that: The guide body (26) comprises a gradually expanding section whose cross section gradually increases in the axial downward direction, and the small end of the gradually expanding section is connected to the bottom end of the central column (24); Preferably, the gradually expanding section is configured to be truncated cone-shaped, and the connection surface between the gradually expanding section and the center column (24) is located above, below or flush with the bottom end surface of the lower vortex chamber (23), and the distance between the connection surface and the bottom end surface of the lower vortex chamber (23) in the height direction is 0 to 0.1 times the diameter of the bottom end of the center column (24).

3. The swirl nozzle according to claim 2, characterized in that: A tapering section whose cross section gradually decreases axially downward is provided below the gradually expanding section; the tapering section is provided in a conical shape; Preferably, a buffer section is provided between the gradually contracting section and the gradually expanding section; More preferably, the buffer section is cylindrical or drum-shaped with a raised center.

4. The swirl nozzle according to claim 1, characterized in that: The nozzle feed inlet (21) is connected to the peripheral wall of the shell and communicates with the upper swirl chamber (22), and the nozzle feed inlet (21) extends along the tangent direction, involute direction or helical direction of the inner peripheral wall of the shell; and / or An angle β between a line connecting an intersection point of a first inner wall (211) of the nozzle feed port (21) and an inner peripheral wall of the shell and a center of the shell and a tangent line to the intersection point is 60° to 120°; and / or The normal cross-section of the nozzle feed port (21) in the material flow direction is one of rectangular, circular or elliptical; and / or The upper swirl chamber (22) is a cylindrical or truncated cone-shaped chamber; Preferably, the ratio of the height of the cylindrical cavity and / or the truncated cone cavity to the diameter of the circle at the middle position is 0.1 to 10; More preferably, the ratio of the maximum diameter to the minimum diameter of the truncated cone cavity is 0.1 to 10; and / or The lower vortex chamber (23) is configured as a tapered chamber that tapers downward, the bottom end of the tapered chamber being formed with the bottom end opening, the top end diameter of the tapered chamber being the same as the bottom end diameter of the upper vortex chamber (22), and the ratio of the bottom end diameter to the top end diameter of the tapered chamber being 0.1 to 10.

5. A tubular distributor, characterized in that: The tubular distributor (4) comprises a branch pipe (13) and a plurality of branch pipes (14) connected to the branch pipe (13), a plurality of swirl nozzles (19) according to any one of claims 1 to 4 being installed on the branch pipe (14), and a rectifying component (16) capable of strengthening the distribution of logistics is provided at the connecting end between the branch pipe (14) and the branch pipe (13).

6. The tubular distributor according to claim 5, characterized in that: The tubular distributor (4) is a tree-branch type tubular distribution structure; a plurality of branch pipes (14) are arranged on both sides of the branch pipe (13); Preferably, the branch pipe (14) is arranged to extend radially along the branch pipe (13), one end of the branch pipe (14) is connected to the side of the branch pipe (13) through a rectifying component (16), and the other end is arranged to be closed; and / or The cross section of the branch pipe (14) is circular, elliptical or rectangular.

7. The tubular distributor according to claim 5 or 6, characterized in that: Along the main flow direction (15) of the logistics, the branch pipe (13) is a tapered pipe with a gradually decreasing lumen cross section; Preferably, the branch pipe (13) is a round pipe, and the ratio of the diameter of the large end to the diameter of the small end of the round pipe is 0.1 to 0.9; More preferably, the branch pipe (13) is composed of multiple sections of circular pipes with different diameters connected end to end; Further optimization; The length of each section of the circular pipe accounts for 0.05 to 0.95 of the total length of the branch pipe (13); and / or The ratio of the maximum diameter to the minimum diameter of the branch pipe (13) is 0.1 to 0.

9.

8. The tubular distributor according to any one of claims 5 to 7, characterized in that: The tubular distributor (4) further comprises a main pipe (12), a plurality of branch pipes (13) are provided, and the plurality of branch pipes (13) are radially 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 set to be closed.

9. The tubular distributor according to claim 5 or 6, characterized in that: The rectifying component (16) is a pipe with a variable diameter, the large end of the rectifying component (16) is connected to the branch pipe (13) in the radial direction, and the small end is connected to the branch pipe (14); Preferably, the tube shell surrounding the rectifying member (16) is composed of a straight tube shell (17) and a different-diameter curved tube shell (18); More preferably, The included 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°; and / or Along the flow direction in the rectifying component (16), the profile of the different-diameter curved tube shell (18) is in the shape of a circular arc, an elliptical arc or a parabola.

10. A fluidized bed reaction device, characterized in that: The fluidized bed reaction device comprises a reaction chamber (2), wherein a material distributor is arranged in the reaction chamber (2), and the material distributor comprises a tubular distributor (4) according to any one of claims 5 to 9; Preferably, The material distributor comprises at least one of the tubular distributors (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.

11. Use of the swirl nozzle according to any one of claims 1 to 4, the tubular distributor according to any one of claims 5 to 9, or the fluidized bed reaction device according to claim 10 in hydrocarbon ammoxidation, catalytic cracking, nitrobenzene hydrogenation or coal gasification reactions.

12. A method for ammoxidation of hydrocarbons, characterized in that: The method adopts the fluidized bed reaction device according to claim 10, wherein the material distributor comprises at least one of the tubular distributors (4) and a gas distribution plate (7); Preferably, the method comprises: The raw material containing the hydrocarbon source and the ammonia source enters the reaction chamber (2) through the tubular distributor (4), and the oxygen-containing gas enters the reaction chamber (2) through the gas distribution plate (7); In the reaction chamber, the raw material containing the hydrocarbon source and the ammonia source is contacted and reacted with the oxygen-containing gas. Preferably, the raw material containing the hydrocarbon source and the ammonia source is contacted and reacted with the oxygen-containing gas in reverse direction.

13. The method according to claim 12, wherein: The unevenness of the spray flow rate of the tubular distributor (4) is 0 to 0.35; and / or The molar ratio of the hydrocarbon source in terms of hydrocarbon groups, the ammonia source in terms of amino groups and the oxygen-containing gas in terms of oxygen molecules is 1:(1-10):(10-40); Preferably, the hydrocarbon source comprises hydrocarbons and / or hydrocarbon derivatives, more preferably comprises at least one of toluene, p-chlorotoluene, o-chlorotoluene, o-xylene, m-xylene, p-xylene, dichlorotoluene, trichlorotoluene and 4-nitro-o-xylene; and / or The ammonia source is ammonia gas; and / or The contact conditions include: reaction temperature of 300-500° C., pressure of 0.01-0.2 MPa, and gas superficial velocity of 0.1-0.8 m / s.

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