Process and apparatus for the oxidative coupling of methane and oxygen-containing gas to produce carbon dihydrides and applications

Abstract

The present application relates to the technical field of petroleum chemical industry, and discloses a method for preparing carbon dihydrocarbon by oxidative coupling of methane and oxygen-containing gas, a device and application thereof.The method comprises the following steps: S1, in the presence of a chrysanthemum petal-shaped diffuser, methane and oxygen-containing gas are contacted by countercurrent diffusion to obtain a mixed gas; S2, under the action of a catalyst, the mixed gas is subjected to oxidative coupling reaction; wherein the molar ratio of the methane to the oxygen-containing gas calculated based on oxygen is 2-15:1.The method can ensure that the raw materials of methane and oxygen-containing gas can be safely fed in large scale, and improve the methane conversion rate, the selectivity of carbon dihydrocarbon and the carbon dihydrocarbon yield.

Description

Technical Field

[0001] This invention relates to the field of petrochemical technology, specifically to a method, apparatus, and application for the oxidative coupling of methane and oxygen-containing gases to prepare C2 hydrocarbons. Background Technology

[0002] Oxidative coupling of methane is an important non-petroleum route for ethylene production. Due to its short reaction process and good economic advantages, it has become a research hotspot in the direct conversion of natural gas. For the reaction process, the mixing of methane and oxygen as feedstocks is a pressing problem. Researchers have found that when methane is activated by oxygen as an oxidant, the ratio of methane to oxygen in the feed directly affects the selectivity and yield of ethylene. When the oxygen content in the feed is high, the methane conversion rate is high, but the corresponding increase in carbon monoxide and carbon dioxide generated by deep oxidation leads to a decrease in the selectivity of ethylene and ethane. Conversely, when the oxygen content in the feed is low, the reaction conversion rate is low due to insufficient oxygen. When the feed rate is small, methane and oxygen can be mixed rapidly, staying away from the explosion limits of methane and oxygen. However, when the feed rates of methane and oxygen increase, the design of industrial plants presents significant challenges. How to achieve safe and rapid mixing while maintaining a high methane conversion rate and reducing the selectivity of carbon dioxide in the product, thus achieving high selectivity and yield of ethylene, has become a key research objective. Summary of the Invention

[0003] The purpose of this invention is to overcome the problems of existing technologies, such as the inability to achieve safe and rapid mixing during large-scale feeding, high carbon dioxide content in the product, and low selectivity and yield of ethylene. This invention provides a method, apparatus, and application for the oxidative coupling of methane and oxygen-containing gas to prepare C2 hydrocarbons. This method can improve the methane conversion rate, C2 hydrocarbon selectivity, and C2 hydrocarbon yield while ensuring safe large-scale feeding of raw materials methane and oxygen-containing gas.

[0004] To achieve the above objectives, the first aspect of the present invention provides a method for preparing C2 hydrocarbons by oxidative coupling of methane and an oxygen-containing gas, characterized in that the method comprises the following steps:

[0005] S1. In the presence of a chrysanthemum petal-shaped diffuser, methane and oxygen-containing gas are subjected to countercurrent diffusion to obtain a mixed gas.

[0006] S2. Under the action of a catalyst, the mixed gas undergoes an oxidative coupling reaction to obtain a C2 hydrocarbon;

[0007] The molar ratio of methane to oxygen-containing gas is 2-15:1.

[0008] A second aspect of the present invention provides an apparatus for the oxidative coupling of methane and oxygen-containing gas to prepare C2 hydrocarbons, characterized in that the apparatus comprises a first inlet pipe 1, a second inlet pipe 2, a mixer 3 and a reactor 4;

[0009] The mixer 3 is provided with a first air inlet pipe 1 and a second air inlet pipe 2, which are used to make the first gas from the first air inlet pipe 1 and the second gas from the second air inlet pipe 2 come into countercurrent diffusion contact and mix.

[0010] The end outlet of the first air inlet pipe 1 is provided with a chrysanthemum petal-shaped diffuser, which is used to diffuse the first gas and send it into the mixer 3, where it is mixed with the second gas;

[0011] The inlet of the reactor 4 is connected to the outlet of the mixer 3, and is used to carry out an oxidative coupling reaction of the mixed gas.

[0012] The reactor 4 is equipped with a catalyst;

[0013] The first intake pipe 1 and the second intake pipe 2 are each used independently to introduce oxygen-containing gas and methane;

[0014] The molar ratio of methane to oxygen-containing gas is 2-15:1.

[0015] The third aspect of the present invention provides the application of the method provided in the first aspect and the apparatus provided in the second aspect in the oxidative coupling reaction of methane.

[0016] Through the above technical solutions, the method, apparatus and application for preparing C2 hydrocarbons by oxidative coupling of methane and oxygen-containing gas provided by the present invention achieve the following beneficial effects: the method can improve the methane conversion rate, C2 hydrocarbon selectivity and C2 hydrocarbon yield while ensuring the safe feeding of raw materials methane and oxygen-containing gas on a large scale. Attached Figure Description

[0017] Figure 1 This is a schematic diagram of the apparatus for preparing C2 hydrocarbons by oxidative coupling of methane and oxygen-containing gas provided in Embodiment 1 of the present invention.

[0018] Explanation of reference numerals in the attached figures

[0019] 1. First air inlet pipe; 2. Second air inlet pipe; 3. Mixer; 4. Reactor; 5. Separator;

[0020] 6. Compressor; 7. Nitrogen; 8. Mixture of ethylene and ethane; 9. Unreacted methane. Detailed Implementation

[0021] 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.

[0022] The first aspect of this invention provides a method for preparing C2 hydrocarbons by oxidative coupling of methane and an oxygen-containing gas, characterized in that the method includes the following steps:

[0023] S1. In the presence of a chrysanthemum petal-shaped diffuser, methane and oxygen-containing gas are subjected to countercurrent diffusion to obtain a mixed gas.

[0024] S2. Under the action of a catalyst, the mixed gas undergoes an oxidative coupling reaction to obtain C2 hydrocarbons;

[0025] The molar ratio of methane to oxygen-containing gas is 2-15:1.

[0026] In this invention, the chrysanthemum petal mixer can diffuse oxygen-containing gas and make countercurrent diffusion contact with methane, so that the mixing ratio of methane and oxygen-containing gas is far away from the explosion zone when heated.

[0027] In this invention, the C2 hydrocarbon is the product of the coupling reaction of methane and oxygen: ethylene and ethane.

[0028] In this invention, the method further includes separating the product after the mixed gas undergoes an oxidative coupling reaction to obtain a mixture of ethylene and ethane, and then separating the mixture to obtain ethylene and ethane respectively.

[0029] In this invention, there are no particular limitations on the separation method and conditions; any separation method conventional in the art can be used.

[0030] In this invention, the catalyst is not particularly limited and can be a conventional catalyst type in the art. Those skilled in the art can adjust it as needed.

[0031] According to the present invention, the molar ratio of methane to oxygen-containing gas is 5-8:1.

[0032] In this invention, the molar ratio of methane to oxygen-containing gas further satisfies the above range, thereby achieving a higher yield of C2 hydrocarbons.

[0033] According to the present invention, the blades of the chrysanthemum petal-shaped diffuser are 1-6 layers.

[0034] In this invention, the number of blade layers of the chrysanthemum petal-shaped diffuser meets the above-mentioned range, which can increase the feed rate and is more suitable for industrial applications.

[0035] Furthermore, the blades of the chrysanthemum petal-shaped diffuser are in 1-3 layers.

[0036] According to the present invention, the number of single-layer blades of the chrysanthemum petal-shaped diffuser is 4-16.

[0037] In this invention, when the number of single-layer blades of the chrysanthemum petal-shaped diffuser meets the above-mentioned range, it can improve the dispersion of the gas, so that the mixture of methane and oxygen-containing gas is far away from the explosion point area when it reacts.

[0038] In this invention, the number of leaves in each layer of the chrysanthemum petal-shaped diffuser is not particularly limited; the number of leaves in each layer can be the same or different.

[0039] Furthermore, the number of single-layer blades of the chrysanthemum petal-shaped diffuser is 8-12.

[0040] According to the present invention, the blades of the chrysanthemum petal-shaped diffuser are hollow thin tubes with an inner diameter of 1-8 mm, preferably 1-4 mm.

[0041] In this invention, the wall thickness of the hollow tube is 0.5-1 mm.

[0042] According to the present invention, the length of the blades of the chrysanthemum petal-shaped diffuser is 1-8 mm.

[0043] In this invention, the length of the blades of the chrysanthemum petal-shaped diffuser meets the above-mentioned range, which enables the mixed gas to quickly reach a state of uniform mixing.

[0044] Furthermore, the blades of the chrysanthemum petal-shaped diffuser are 2-3 mm in length.

[0045] According to the present invention, the space velocity of the methane is 50-50000 mL / min, preferably 50-40000 mL / min.

[0046] According to the present invention, the method further includes preheating the mixed gas before carrying out the oxidative coupling reaction.

[0047] According to the present invention, the preheating conditions include: a preheating temperature of 50-600°C, preferably 50-450°C.

[0048] According to the present invention, the conditions for the oxidative coupling reaction include: a reaction temperature of 450-900°C, preferably 450-750°C.

[0049] According to the present invention, the conditions for the oxidative coupling reaction include: a reaction pressure not greater than 0.7 MPa, preferably not greater than 0.4 MPa.

[0050] According to the present invention, when the mixed gas undergoes an oxidative coupling reaction, liquid metal is used as the heat removal medium.

[0051] In this invention, liquid metal is used as a heat removal medium, which can ensure that the heat released during the reaction can be effectively removed, improve process safety, and ensure the yield and selectivity of the product C2 hydrocarbon.

[0052] According to the present invention, the liquid metal is selected from at least one of low-melting-point metals.

[0053] A second aspect of the present invention provides an apparatus for the oxidative coupling of methane and oxygen-containing gas to prepare C2 hydrocarbons, characterized in that the apparatus comprises a first inlet pipe 1, a second inlet pipe 2, a mixer 3 and a reactor 4;

[0054] The mixer 3 is provided with a first air inlet pipe 1 and a second air inlet pipe 2, which are used to make the first gas from the first air inlet pipe 1 and the second gas from the second air inlet pipe 2 come into countercurrent diffusion contact and mix.

[0055] The end outlet of the first air inlet pipe 1 is provided with a chrysanthemum petal-shaped diffuser, which is used to diffuse the first gas and send it into the mixer 3, where it is mixed with the second gas;

[0056] The inlet of the reactor 4 is connected to the outlet of the mixer 3, and is used to carry out an oxidative coupling reaction of the mixed gas.

[0057] The reactor 4 is equipped with a catalyst;

[0058] The first intake pipe 1 and the second intake pipe 2 are each used independently to introduce oxygen-containing gas and methane;

[0059] The molar ratio of methane to oxygen-containing gas is 2-15:1.

[0060] In this invention, it should be noted that the device described herein may contain multiple first air inlet pipes 1, multiple second air inlet pipes 2, and multiple mixers 3. In industrial applications, depending on the amount of gas entering the system, a single first air inlet pipe 1, a single second air inlet pipe 2, and a single mixer 3 can be used as an independent mixing unit. Multiple mixing units can be connected in parallel to simultaneously complete large-scale gas mixing while ensuring relative isolation between the individual chrysanthemum petal diffusers. This ensures that if a local deflagration occurs in a single mixing unit during gas mixing, it will not affect other mixing units, thereby improving process stability, safety, and continuity.

[0061] In this invention, the molar ratio of methane to oxygen-containing gas is further 5-8:1.

[0062] In this invention, the methane and oxygen-containing materials are mixed at room temperature and then fed into reactor 4. There is no particular limitation on the type of reactor 4, such as a fixed bed, fluidized bed, or boiling bed. The reactor 4 is filled with a catalyst, and both the upper and lower ends of the catalyst are filled with inert materials.

[0063] Furthermore, there is no particular limitation on the type of inert material, such as quartz sand.

[0064] According to the present invention, the height of the mixer 3 is H, and the mixing point of the methane and the oxygen-containing gas is 1 / 3H-1 / 2H from top to bottom of the mixer 3, preferably 1 / 3H-2 / 5H.

[0065] In this invention, the mixer 3 is a stainless steel round tube with a wall thickness of 1-2 mm, the inner diameter of the stainless steel round tube is 12-36 mm, preferably 12-18 mm, and the length is not less than 500 mm.

[0066] According to the present invention, the angle between the blades of the chrysanthemum petal-shaped diffuser at the end outlet of the first air intake pipe 1 and the central axis of the first air intake pipe 1 is 45°-100°.

[0067] In this invention, the angle between the blades of the chrysanthemum petal-shaped diffuser at the end outlet of the first air intake pipe 1 and the central axis of the first air intake pipe 1 satisfies the above-mentioned range, which enables the mixed gas to be mixed quickly and evenly.

[0068] According to the present invention, the angle between the blades of the chrysanthemum petal-shaped diffuser at the end outlet of the first air intake pipe 1 and the central axis of the first air intake pipe 1 is 50°-90°.

[0069] Combination Figure 1 A specific embodiment of the method provided in the first aspect of the present invention in the apparatus provided in the second aspect (taking air being introduced into the first air intake pipe 1 as an example) includes:

[0070] S1. The mixer 3 with a height of H is provided with a first air inlet pipe 1 and a second air inlet pipe 2, which are used to bring oxygen-containing gas from the first air inlet pipe 1 and methane (space velocity of 50-5000 mL / min) from the second air inlet pipe 2 into countercurrent contact at 1 / 3H-1 / 2H from top to bottom in the mixer 3 to obtain a mixed gas (molar ratio of methane to oxygen-containing gas is 2-15:1);

[0071] S2. The inlet of the reactor 4 is connected to the outlet of the mixer 3, which is used to preheat the mixed gas at a temperature of 50-600℃ and carry out an oxidative coupling reaction at a temperature of 450-900℃ and a pressure of no more than 0.7MPa in the presence of a catalyst, and liquid metal is provided as a heat removal medium.

[0072] The chrysanthemum petal-shaped diffuser has 1-6 layers of blades, with 4-16 blades per layer, a blade length of 1-8 mm, and an inner diameter of 1-8 mm for the hollow tube.

[0073] The angle between the blades of the chrysanthemum petal-shaped diffuser at the end outlet of the first air intake pipe 1 and the central axis of the first air intake pipe 1 is 45-100°.

[0074] The third aspect of the present invention provides the application of the method provided in the first aspect and the apparatus provided in the second aspect in the oxidative coupling reaction of methane.

[0075] The present invention will be described in detail below through examples. In the following examples, the analysis of the reaction product components was performed on a gas chromatograph, model 7890A, purchased from Agilent Technologies.

[0076] The method for calculating methane conversion rate is as follows:

[0077] Methane conversion rate = Total methane consumption / Initial amount of methane × 100%.

[0078] The method for calculating ethylene selectivity is as follows:

[0079] Ethylene selectivity = Amount of methane consumed to produce ethylene / Total methane consumption × 100%.

[0080] The method for calculating ethane selectivity is as follows:

[0081] Ethane selectivity = Amount of methane consumed to produce ethane / Total methane consumption × 100%.

[0082] C2 hydrocarbon selectivity = ethylene selectivity + ethane selectivity.

[0083] The method for calculating the yield of C2 hydrocarbons is as follows:

[0084] C2 hydrocarbon yield = methane conversion rate × C2 hydrocarbon selectivity.

[0085] Example 1

[0086] S1. The mixer 3 with a height of H is provided with a first air inlet pipe 1 and a second air inlet pipe 2, which are used to bring oxygen-containing gas from the first air inlet pipe 1 and methane (space velocity of 30000 mL / min) from the second air inlet pipe 2 into countercurrent contact at a distance of 20 cm (1 / 2H) from top to bottom in the mixer 3 to obtain a mixed gas (molar ratio of methane to oxygen-containing gas is 5:1);

[0087] S2. The inlet of the reactor 4 is connected to the outlet of the mixer 3, which is used to preheat the mixed gas at a temperature of 200°C and carry out an oxidative coupling reaction at a temperature of 700°C and a pressure of 0.03MPa in the presence of lanthanum oxide catalyst. Liquid tin metal is provided as a heat removal medium, and finally the oxidative coupling products are separated to obtain ethylene and ethane.

[0088] The chrysanthemum petal-shaped diffuser has two layers of blades, with eight blades per layer, a blade length of 2 mm, and an inner diameter of 2 mm for the hollow tube.

[0089] The angle between the blades of the chrysanthemum petal-shaped diffuser at the end outlet of the first air intake pipe 1 and the central axis of the first air intake pipe 1 is 90°.

[0090] The conversion rate of methane, the selectivity of C2 hydrocarbons, and the yield are shown in Table 1.

[0091] Example 2

[0092] The method is consistent with that in Example 1, except that the chrysanthemum petal diffuser has two layers of blades, with 12 blades per layer, and the molar ratio of methane to oxygen-containing gas is 8:1. The final methane conversion rate, C2 hydrocarbon selectivity, and C2 hydrocarbon yield are shown in Table 1.

[0093] Example 3

[0094] The method is consistent with that in Example 1, except that the inner diameter of the hollow tube is 1 mm, and a mixed gas is obtained, wherein the molar ratio of methane to oxygen-containing gas is 6:1. The final methane conversion rate, C2 hydrocarbon selectivity and yield are shown in Table 1.

[0095] Example 4

[0096] The method is consistent with that in Example 1, except that the blades of the chrysanthemum petal-shaped diffuser are 3 mm long, resulting in a mixed gas in which the molar ratio of methane to oxygen-containing gas is 7:1. The final methane conversion, C2 hydrocarbon selectivity, and yield are shown in Table 1.

[0097] Example 5

[0098] The method is consistent with that in Example 1, except that the number of blades in the chrysanthemum petal diffuser is 4, the molar ratio of methane to oxygen-containing gas is 3:1, and the final methane conversion, C2 hydrocarbon selectivity and yield are shown in Table 1.

[0099] Example 6

[0100] The method is consistent with that in Example 1, except that the angle between the blades of the chrysanthemum petal-shaped diffuser at the end outlet of the first intake pipe 1 and the central axis of the first intake pipe 1 is 100°, the molar ratio of methane to oxygen-containing gas is 2:1, and the final methane conversion rate, C2 hydrocarbon selectivity and yield are shown in Table 1.

[0101] Example 7

[0102] The method is consistent with that in Example 1, except that the inner diameter of the hollow tube is 9 mm, the molar ratio of methane to oxygen-containing gas is 16:1, and the final methane conversion, C2 hydrocarbon selectivity and yield are shown in Table 1.

[0103] Example 8

[0104] The method is consistent with that in Example 1, except that methane (space velocity 4000 mL / min) is countercurrently contacted at a distance of 40 cm (2 / 3H) from top to bottom in mixer 3 to obtain a mixed gas (methane and oxygen-containing gas molar ratio of 5:1). The final methane conversion, C2 hydrocarbon selectivity and yield are shown in Table 1.

[0105] Comparative Example 1

[0106] The method is consistent with that of Example 1, except that the number of single-layer blades of the chrysanthemum petal diffuser is 17, so that the molar ratio of methane to oxygen-containing gas in the mixed gas is 16:1. The final methane conversion rate, C2 hydrocarbon selectivity, and C2 hydrocarbon yield are shown in Table 1.

[0107] Table 1

[0108] Example 1 25.6 33.5 20.1 53.6 13.72 Example 2 26.3 32.1 22.1 54.2 14.25 Example 3 26.5 35.6 18.3 53.9 14.28 Example 4 24.3 34.6 15.5 50.1 12.17 Example 5 23.7 33.5 15.1 48.6 11.52 Example 6 22.5 32.1 15.7 47.8 10.76 Example 7 21.6 36.5 9.8 46.3 10 Example 8 20.5 33.2 12.6 45.8 9.39 Comparative Example 1 12.3 21.2 22.4 43.6 5.36

[0109] As can be seen from the results in Table 1, the use of Examples 1-8 of the present invention has good effects, with the conversion rate of methane all above 20%, while the selectivity of C2 hydrocarbons is not less than 45% and the yield of C2 hydrocarbons is not less than 9%.

[0110] Furthermore, Examples 1-4, which satisfy the preferred technical solutions of the present invention, have significantly better effects, with alkane conversion rates all above 24%, while C2 hydrocarbon selectivity is not less than 50% and C2 hydrocarbon yield is not less than 12%.

[0111] The preferred embodiments of the present invention have been described in detail above; 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 technical features in any other suitable manner. 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 method for preparing C2 hydrocarbons by oxidative coupling of methane and oxygen-containing gas, characterized in that, The method includes the following steps: S1. In the presence of a chrysanthemum petal-shaped diffuser, methane and oxygen-containing gas are subjected to countercurrent diffusion to obtain a mixed gas; the oxygen-containing gas is introduced into the chrysanthemum petal-shaped diffuser. S2. Under the action of a catalyst, the mixed gas undergoes an oxidative coupling reaction to obtain C2 hydrocarbons; The molar ratio of methane to oxygen-containing gas is 5-8:

1. The chrysanthemum petal-shaped diffuser has 2-6 layers of blades; The blades of the chrysanthemum petal-shaped diffuser are hollow thin tubes with an inner diameter of 1-8 mm. The blades of the chrysanthemum petal-shaped diffuser are 1-8 mm in length.

2. The method according to claim 1, wherein, The chrysanthemum petal-shaped diffuser has 2-3 layers of blades and / or the number of blades in a single layer of the chrysanthemum petal-shaped diffuser is 4-16.

3. The method according to claim 2, wherein, The number of blades in a single layer of the chrysanthemum petal-shaped diffuser is 8-12.

4. The method according to any one of claims 1-3, wherein, The inner diameter of the hollow tube is 1-4 mm; And / or, the length of the blades of the chrysanthemum petal-shaped diffuser is 2-3 mm.

5. The method according to any one of claims 1-3, wherein, The space velocity of the methane is 50-50000 mL / min.

6. The method according to claim 5, wherein, The space velocity of the methane is 50-40000 mL / min.

7. The method according to any one of claims 1-3, wherein, The method further includes preheating the mixed gas before carrying out the oxidative coupling reaction.

8. The method according to claim 7, wherein, The preheating conditions include a preheating temperature of 50-600℃.

9. The method according to claim 8, wherein, The preheating conditions include a preheating temperature of 50-450℃.

10. The method according to any one of claims 1-3, wherein, The conditions for the oxidative coupling reaction include: a reaction temperature of 450-900℃; and a reaction pressure of no more than 0.7 MPa.

11. The method according to claim 10, wherein, The conditions for the oxidative coupling reaction include: a reaction temperature of 450-750℃; and a reaction pressure of no more than 0.4 MPa.

12. The method according to any one of claims 1-3, wherein, When the mixed gas undergoes an oxidative coupling reaction, liquid metal is used as the heat removal medium.

13. The method according to claim 12, wherein, The liquid metal is selected from at least one of low-melting-point metals.

14. An apparatus for the oxidative coupling of methane and an oxygen-containing gas to prepare C2 hydrocarbons, characterized in that, The device includes a first air inlet pipe (1), a second air inlet pipe (2), a mixer (3), and a reactor (4); The mixer (3) is provided with a first air inlet pipe (1) and a second air inlet pipe (2) for countercurrent diffusion contact and mixing of the first gas from the first air inlet pipe (1) and the second gas from the second air inlet pipe (2); The first intake pipe (1) is provided with a chrysanthemum petal-shaped diffuser at its end outlet, which is used to diffuse the first gas and send it into the mixer (3) to mix with the second gas; The inlet of the reactor (4) is connected to the outlet of the mixer (3) for oxidative coupling reaction of the mixed gas; The reactor (4) is equipped with a catalyst; The first intake pipe (1) and the second intake pipe (2) are each used independently to introduce oxygen-containing gas and methane; The molar ratio of methane to oxygen-containing gas is 5-8:

1. The chrysanthemum petal-shaped diffuser has 2-6 layers of blades; The blades of the chrysanthemum petal-shaped diffuser are hollow thin tubes with an inner diameter of 1-8 mm. The blades of the chrysanthemum petal-shaped diffuser are 1-8 mm in length.

15. The apparatus according to claim 14, wherein the mixer (3) has a height of H, and the mixing point of the methane and the oxygen-containing gas is located at 1 / 3H-1 / 2H from top to bottom in the mixer (3); And / or, the angle between the blades of the chrysanthemum petal-shaped diffuser at the end outlet of the first air intake pipe (1) and the central axis of the first air intake pipe (1) is 45°-100°.

16. The use of the method according to any one of claims 1-13 and the apparatus according to claim 14 or 15 in the oxidative coupling reaction of methane.

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