CN111056896B - Reaction system and reaction method for oxide recycling in methanol catalytic conversion process - Google Patents

Abstract

The invention relates to a reaction system and a reaction method for oxide recycling in a methanol catalytic conversion process, and mainly solves the problem of low oxide conversion rate in oxide recycling in the prior art. The invention relates to a technical scheme that a mixed oxide aqueous solution raw material generated by a separation unit in the methanol catalytic conversion process enters a reactor oxide recycling area to be in contact reaction with a regenerated catalyst, the methanol raw material enters a reactor methanol conversion area to be in contact reaction with a spent catalyst, a generated reaction product is separated from the catalyst by a cyclone separator and then enters a subsequent separation system, the spent catalyst enters a regenerator through a spent inclined tube to burn off carbon deposit to obtain the regenerated catalyst, and the regenerated catalyst returns to the reactor oxide recycling area through the regenerated inclined tube.

Description

Reaction system and reaction method for oxide recycling in methanol catalytic conversion process

Technical Field

The invention relates to a reaction system and a reaction method for oxide recycling in a methanol catalytic conversion process.

Background

Light olefins, i.e. ethylene and propylene, are two important basic chemical raw materials, and the demand of the light olefins is increasing. Generally, ethylene and propylene are produced by the petroleum route, but due to the limited supply of petroleum resources, in recent years, technologies for producing ethylene and propylene by conversion of alternative raw materials have been developed greatly. Among them, an important alternative raw material for producing low-carbon olefins is an oxygen-containing compound, such as alcohols (methanol and ethanol), ethers (dimethyl ether and methyl ethyl ether), esters (dimethyl carbonate and methyl formate), and the oxygen-containing compound can be converted from energy sources such as coal, natural gas and biomass. Certain oxygenates have been produced on a larger scale, such as methanol, from coal or natural gas, and the process is well established and can be produced on a megaton scale. Due to the wide availability of oxygenate sources, coupled with the economics of the conversion to lower olefins, processes for the conversion of Oxygenates To Olefins (OTO), particularly Methanol To Olefins (MTO), have received increasing attention.

The application of silicoaluminophosphate molecular sieve catalyst to a process for preparing olefin by methanol conversion is studied in detail in the patent of US4499327, and SAPO-34 is considered to be the first catalyst for MTO process. The SAPO-34 catalyst has high selectivity and high activity for low-carbon olefin, and can ensure that the reaction time for converting methanol into the low-carbon olefin reaches a degree of less than 10 seconds, even reaches the reaction time range of a riser.

US6166282 discloses a technology and reactor for converting methanol into low carbon olefins, which uses a fast fluidized bed reactor, after the gas phase is reacted in a dense phase reaction zone with a lower gas velocity, the gas phase rises to a fast partition zone with a rapidly decreasing inner diameter, and a special gas-solid separation device is used for primarily separating most entrained catalyst. Because the product gas and the catalyst are quickly separated after the reaction, the occurrence of secondary reaction is effectively prevented. Through simulation calculation, compared with the traditional bubbling fluidized bed reactor, the internal diameter of the fast fluidized bed reactor and the required inventory of the catalyst are both greatly reduced.

CN1723262 discloses a multi-stage riser reactor with a central catalyst loop for converting oxides into lower olefins, which comprises multiple riser reactors, a gas-solid separation zone, multiple offset elements, etc., wherein each of the riser reactors has a port for injecting catalyst, and converges to the separation zone to separate the catalyst from the product gas.

In order to reduce the carbon-based loss of raw materials, the prior art directly returns the oxygen-containing compounds and unconverted methanol to an MTO reactor. However, the prior art has the problems of low conversion rate of the byproduct oxide and need of large amount of external throwing, and the patent aims to solve the problems.

Disclosure of Invention

The invention aims to solve the technical problem that the oxide conversion rate is low during oxide recycling in the prior art, and provides a reaction system for oxide recycling in a methanol catalytic conversion process. The system has the advantage of high oxide conversion rate during oxide recycling.

The second technical problem to be solved by the present invention is to provide a reaction method corresponding to the first technical problem.

In order to solve one of the problems, the technical scheme adopted by the invention is as follows: the reaction system for oxide recycling in the catalytic conversion process of methanol is provided, and comprises a dense-phase section (1) of a reactor, a dilute-phase section (2) of the reactor, an oxide recycling area (3) of the reactor, a methanol conversion area (4) of the reactor, a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a to-be-regenerated inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

In the technical scheme, the partition plate (9) consists of a porous area (12) and a non-porous area (13), the porous area (12) is positioned above the non-porous area (13), an included angle alpha between the porous area (12) and the non-porous area (13) ranges from 120 degrees to 160 degrees, the aperture ratio of the porous area (12) is 50-80%, and the area ratio of the porous area (12) to the non-porous area (13) is (0.5-3): 1; the height of the partition (9) accounts for 50-80% of the total height of the dense-phase section (1) of the reactor.

In the above technical solution, preferably, an included angle α between the porous region (12) and the non-porous region (13) ranges from 130 ° to 150 °, an aperture ratio of the porous region (12) is 65 to 80%, and a ratio of areas of the porous region (12) and the non-porous region (13) is (1 to 2): 1; the height of the partition (9) accounts for 60-80% of the total height of the dense-phase section (1) of the reactor.

In the technical scheme, preferably, the partition (9) is a vertical non-porous plate, and the height of the partition (9) accounts for 30-50% of the total height of the dense-phase section (1) of the reactor.

In the technical scheme, preferably, the partition (9) is a vertical non-porous plate, and the height of the partition (9) accounts for 35-45% of the total height of the dense-phase section (1) of the reactor.

In the above technical solution, preferably, the two partition plates (9) are arranged in parallel, the area between the two partition plates (9) is a reactor methanol conversion area (4), and the reactor oxide recycling area is divided into a reactor oxide recycling area I (3-1) and a reactor oxide recycling area II (3-2).

In the technical scheme, preferably, the volume ratio of the methanol conversion zone (4) of the reactor to the oxide recycling zone (3) of the reactor is (3-10): 1.

In order to solve the second problem, the invention adopts the following technical scheme: a reaction method for oxide recycling in a methanol catalytic conversion process comprises the following steps:

a) mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10);

b) the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6);

c) the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide remixing area (3) of the reactor through a regenerated inclined tube (5).

In the above technical scheme, preferably, the mixed oxide in the mixed oxide aqueous solution raw material (8) is 5-70% by weight, the mixed oxide contains at least one of methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid, and propionic acid, and the ketones in the mixed oxide are 30-80% by weight.

In the technical scheme, preferably, the temperature of the catalyst bed layer in the oxide recycling area (3) of the reactor is 480-680 ℃, the density of the catalyst is 70-150 kg/cubic meter, and the gas velocity is 0.8-1.5 m/s.

In the technical scheme, preferably, the temperature of a catalyst bed layer in the methanol conversion zone (4) of the reactor is 450-550 ℃, the density of the catalyst is 200-500 kg/cubic meter, and the gas velocity is 0.5-1.5 m/s.

In the above technical solution, preferably, the carbon content of the regenerated catalyst (10) is less than 0.1% by total mass of the catalyst.

According to the technical scheme for oxide recycling in the methanol catalytic conversion process, the MTO fluidized bed reactor is divided into an oxide recycling area and a methanol conversion area, so that the very high oxide conversion rate is favorably obtained, the oxide can be efficiently converted into low-carbon hydrocarbon, and the generation of heavy hydrocarbon and phenol compounds is avoided. By adopting the technical scheme of the invention, the conversion rate of the oxide is 100 percent by weight calculated by acetone; the total yield of ethylene and propylene carbon is up to 84.6 wt%, and good technical effect is obtained.

Drawings

FIG. 1 is a schematic diagram of an apparatus of a reaction system for oxide recycle in a methanol catalytic conversion process according to the present invention, wherein one partition plate is provided.

FIG. 2 is a schematic view of a separator, 12 being a porous region; and 13 is a non-porous area.

FIG. 3 is a schematic view of another apparatus of the reaction system for oxide recycle in the methanol catalytic conversion process according to the present invention, in which two partitions are provided.

In the figure, 1 is a dense-phase section of the reactor; 2 is a reactor dilute phase section; 3 is a reactor oxide recycling zone; 4 is a methanol conversion zone of the reactor; 5 is a regeneration inclined tube; 6 is a cyclone separator; 7 is a methanol raw material; 8 is a mixed oxide aqueous solution raw material; 9 is a clapboard; 10 is a regenerated catalyst; 11 is a reaction product; 14 is a to-be-grown inclined tube; 15 is spent catalyst.

The present invention will be further illustrated by the following examples, but is not limited to these examples.

Detailed Description

[ example 1 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the inclined tube to be generated (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition board (9) is composed of a porous area (12) and a non-porous area (13), the porous area (12) is positioned above the non-porous area (13), the included angle alpha between the porous area (12) and the non-porous area (13) ranges from 120 degrees, the aperture ratio of the porous area (12) is 80 percent, and the area ratio of the porous area (12) to the non-porous area (13) is 0.5: 1; the height of the partition (9) accounts for 50 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 5: 1.

The mixed oxide water solution raw material (8) contains 50% of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 70% of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 550 ℃, the density of the catalyst is 130 kg/cubic meter, and the gas velocity is 1.2 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 470 ℃, the density of the catalyst is 300 kg/cubic meter, and the gas velocity is 0.9 m/s.

The regenerated catalyst (10) had a carbon content of 0.05% based on the total mass of the catalyst.

The results showed an oxide conversion of 87.5 wt% and a combined ethylene and propylene carbon yield of 82.2 wt%.

[ example 2 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The separator (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 160 degrees, the aperture ratio of the porous region (12) is 50%, and the area ratio of the porous region (12) to the non-porous region (13) is 3: 1; the height of the partition (9) accounts for 80 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 5: 1.

The mixed oxide water solution raw material (8) contains 50% of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 70% of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 550 ℃, the density of the catalyst is 130 kg/cubic meter, and the gas velocity is 1.2 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 470 ℃, the density of the catalyst is 300 kg/cubic meter, and the gas velocity is 0.9 m/s.

The regenerated catalyst (10) had a carbon content of 0.05% based on the total mass of the catalyst.

The results showed that the conversion of the oxide was 89.6 wt% and the total yield of carbon based on ethylene and propylene was 83.0 wt%.

[ example 3 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense phase section (1) of the reactor consists of a reactor oxide recycle zone (3) and a reactor methanol conversion zone (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide remixing area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 140 degrees, the aperture ratio of the porous region (12) is 70%, and the area ratio of the porous region (12) to the non-porous region (13) is 1: 1; the height of the partition (9) accounts for 60 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 5: 1.

The mixed oxide water solution raw material (8) contains 50% of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 70% of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 550 ℃, the density of the catalyst is 130 kg/cubic meter, and the gas velocity is 1.2 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 470 ℃, the density of the catalyst is 300 kg/cubic meter, and the gas velocity is 0.9 m/s.

The regenerated catalyst (10) had a carbon content of 0.05% based on the total mass of the catalyst.

The results show an oxide conversion of 94.5 wt% and a combined ethylene and propylene carbon yield of 85.2 wt%.

[ example 4 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 140 degrees, the aperture ratio of the porous region (12) is 70%, and the area ratio of the porous region (12) to the non-porous region (13) is 1: 1; the height of the partition (9) accounts for 60 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 3: 1.

The mixed oxide aqueous solution raw material (8) contains 50% of mixed oxide by mass, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 70% of ketones by mass.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 550 ℃, the density of the catalyst is 130 kg/cubic meter, and the gas velocity is 1.2 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 470 ℃, the density of the catalyst is 300 kg/cubic meter, and the gas velocity is 0.9 m/s.

The regenerated catalyst (10) had a carbon content of 0.05% based on the total mass of the catalyst.

The results showed 92.7 wt% conversion of the oxygenate and 84.7 wt% total yield of carbon based on ethylene and propylene.

[ example 5 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 140 degrees, the aperture ratio of the porous region (12) is 70%, and the area ratio of the porous region (12) to the non-porous region (13) is 1: 1; the height of the partition (9) accounts for 60 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 10: 1.

The mixed oxide water solution raw material (8) contains 50% of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 70% of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 550 ℃, the density of the catalyst is 130 kg/cubic meter, and the gas velocity is 1.2 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 470 ℃, the density of the catalyst is 300 kg/cubic meter, and the gas velocity is 0.9 m/s.

The regenerated catalyst (10) had a carbon content of 0.05% based on the total mass of the catalyst.

The results showed 91.9 wt% conversion of the oxides and 83.8 wt% total yield of carbon based on ethylene and propylene.

[ example 6 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The separator (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 140 degrees, the aperture ratio of the porous region (12) is 70%, and the area ratio of the porous region (12) to the non-porous region (13) is 1: 1; the height of the partition (9) accounts for 60 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 5: 1.

The mixed oxide water solution raw material (8) contains 5% of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 80% of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 550 ℃, the density of the catalyst is 130 kg/cubic meter, and the gas velocity is 1.2 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 470 ℃, the density of the catalyst is 300 kg/m, and the gas velocity is 0.9 m/s.

The regenerated catalyst (10) had a carbon content of 0.05% based on the total mass of the catalyst.

The results show an oxide conversion of 88.6 wt% and a combined ethylene and propylene carbon yield of 82.7 wt%.

[ example 7 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 140 degrees, the aperture ratio of the porous region (12) is 70%, and the area ratio of the porous region (12) to the non-porous region (13) is 1: 1; the height of the partition (9) accounts for 60 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 5: 1.

The mixed oxide in the mixed oxide water solution raw material (8) accounts for 70 percent by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains ketones in 30 percent by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 550 ℃, the density of the catalyst is 130 kg/cubic meter, and the gas velocity is 1.2 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 470 ℃, the density of the catalyst is 300 kg/cubic meter, and the gas velocity is 0.9 m/s.

The regenerated catalyst (10) had a carbon content of 0.05% by mass of the total catalyst.

The results show that the conversion of the oxides is 90.3% by weight and the overall yield of the carbon based ethylene and propylene is 84.1% by weight.

[ example 8 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 140 degrees, the aperture ratio of the porous region (12) is 70%, and the area ratio of the porous region (12) to the non-porous region (13) is 1: 1; the height of the partition (9) accounts for 60 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 5: 1.

The mixed oxide water solution raw material (8) contains 50% of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 70% of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 350 ℃, the density of the catalyst is 150 kg/cubic meter, and the gas velocity is 0.8 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 470 ℃, the density of the catalyst is 300 kg/cubic meter, and the gas velocity is 0.9 m/s.

The regenerated catalyst (10) had a carbon content of 0.05% based on the total mass of the catalyst.

The results showed 91.5 wt% conversion of the oxides and 83.9 wt% total yield of carbon based on ethylene and propylene.

[ example 9 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 140 degrees, the aperture ratio of the porous region (12) is 70%, and the area ratio of the porous region (12) to the non-porous region (13) is 1: 1; the height of the partition (9) accounts for 60 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 5: 1.

The mixed oxide water solution raw material (8) contains 50% of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 70% of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 680 ℃, the density of the catalyst is 70 kg/cubic meter, and the gas velocity is 1.5 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 470 ℃, the density of the catalyst is 300 kg/cubic meter, and the gas velocity is 0.9 m/s.

The regenerated catalyst (10) had a carbon content of 0.05% based on the total mass of the catalyst.

The results showed 92.4 wt% conversion of the oxygenate and 84.3 wt% total yield of carbon based on ethylene and propylene.

[ example 10 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 140 degrees, the aperture ratio of the porous region (12) is 70%, and the area ratio of the porous region (12) to the non-porous region (13) is 1: 1; the height of the partition (9) accounts for 60 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 5: 1.

The mixed oxide water solution raw material (8) contains 50% of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 70% of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 550 ℃, the density of the catalyst is 130 kg/cubic meter, and the gas velocity is 1.2 m/s.

The temperature of the catalyst bed layer in the methanol conversion zone (4) of the reactor is 450 ℃, the density of the catalyst is 500 kg/cubic meter, and the gas velocity is 0.5 m/s.

The regenerated catalyst (10) had a carbon content of 0.05% based on the total mass of the catalyst.

The results show an oxygenate conversion of 92.8 wt.% and a combined ethylene and propylene carbon yield of 82.4 wt.%.

[ example 11 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 140 degrees, the aperture ratio of the porous region (12) is 70%, and the area ratio of the porous region (12) to the non-porous region (13) is 1: 1; the height of the partition (9) accounts for 60 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 5: 1.

The mixed oxide water solution raw material (8) contains 50% of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 70% of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 550 ℃, the density of the catalyst is 130 kg/cubic meter, and the gas velocity is 1.2 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 530 ℃, the density of the catalyst is 200 kg/cubic meter, and the gas velocity is 1.5 m/s.

The regenerated catalyst (10) had a carbon content of 0.05% based on the total mass of the catalyst.

The results showed 92.5 wt% conversion of the oxygenate and 84.7 wt% total yield of carbon based on ethylene and propylene.

[ example 12 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 140 degrees, the aperture ratio of the porous region (12) is 70%, and the area ratio of the porous region (12) to the non-porous region (13) is 1: 1; the height of the partition (9) accounts for 60 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 5: 1.

The mixed oxide water solution raw material (8) contains 50% of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 70% of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 550 ℃, the density of the catalyst is 130 kg/cubic meter, and the gas velocity is 1.2 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 470 ℃, the density of the catalyst is 300 kg/cubic meter, and the gas velocity is 0.9 m/s.

The regenerated catalyst (10) had a carbon content of 0.009% based on the total mass of the catalyst.

The results show that the conversion of the oxides is 86.6% by weight and the overall yield of the carbon based on ethylene and propylene is 82.3% by weight.

[ example 13 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 150 degrees, the aperture ratio of the porous region (12) is 60%, and the area ratio of the porous region (12) to the non-porous region (13) is 2: 1; the height of the partition (9) accounts for 70% of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 500 ℃, the density of the catalyst is 100 kg/cubic meter, and the gas velocity is 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results show an oxide conversion of 93.4 wt% and a combined ethylene and propylene carbon yield of 85.2 wt%.

[ example 14 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined pipe (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The baffle (9) is a vertical non-porous plate, and the height of the baffle (9) accounts for 30 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 500 ℃, the density of the catalyst is 100 kg/cubic meter, and the gas velocity is 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results showed that the conversion of the oxide was 96.8 wt% and the overall yield of the carbon based ethylene and propylene was 83.7 wt%.

[ example 15 ]

The device shown in figure 1 is adopted, and comprises a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The baffle (9) is a vertical non-porous plate, and the height of the baffle (9) accounts for 50 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 500 ℃, the density of the catalyst is 100 kg/cubic meter, and the gas velocity is 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results showed 97.8 wt% conversion of the oxide and 84.3 wt% total yield of carbon based on ethylene and propylene.

[ example 16 ]

Adopting a device shown in figure 3, comprising a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling areas (3-1 and 3-2) of the reactor and the methanol conversion area (4) of the reactor are connected by a partition plate (9), the oxide recycling areas (3-1 and 3-2) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The baffle (9) is a vertical non-porous plate, and the height of the baffle (9) accounts for 40 percent of the total height of the dense-phase section (1) of the reactor.

The two partition plates (9) are arranged in parallel, the area between the two partition plates (9) is a reactor methanol conversion area (4), and the reactor oxide recycling area is divided into a reactor oxide recycling area (3-1) and a reactor oxide recycling area (3-2).

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 500 ℃, the density of the catalyst is 100 kg/cubic meter, and the gas velocity is 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results showed 97.1 wt% conversion of the oxide and 83.7 wt% total yield of carbon based on ethylene and propylene.

[ example 17 ]

Adopting a device shown in figure 3, comprising a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling areas (3-1 and 3-2) of the reactor and the methanol conversion area (4) of the reactor are connected by a partition plate (9), the oxide recycling areas (3-1 and 3-2) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and the generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The baffle (9) is a vertical non-porous plate, and the height of the baffle (9) accounts for 40 percent of the total height of the dense-phase section (1) of the reactor.

The two partition plates (9) are arranged in parallel, the area between the two partition plates (9) is a reactor methanol conversion area (4), and the reactor oxide recycling area is divided into a reactor oxide recycling area (3-1) and a reactor oxide recycling area (3-2).

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 500 ℃, the density of the catalyst is 100 kg/cubic meter, and the gas velocity is 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results showed 97.9 wt% conversion of the oxide and 84.7 wt% total yield of carbon based on ethylene and propylene.

[ example 18 ]

Adopting a device shown in figure 3, comprising a reactor dense-phase section (1), a reactor dilute-phase section (2), a reactor oxide remilling zone (3), a reactor methanol conversion zone (4), a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a spent inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling areas (3-1 and 3-2) of the reactor and the methanol conversion area (4) of the reactor are connected by a partition plate (9), the oxide recycling areas (3-1 and 3-2) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 150 degrees, the aperture ratio of the porous region (12) is 60%, and the area ratio of the porous region (12) to the non-porous region (13) is 2: 1; the height of the partition (9) accounts for 70 percent of the total height of the dense-phase section (1) of the reactor.

The two partition plates (9) are arranged in parallel, the area between the two partition plates (9) is a reactor methanol conversion area (4), and the reactor oxide recycling area is divided into a reactor oxide recycling area (3-1) and a reactor oxide recycling area (3-2).

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide water solution raw material contains 30% of mixed oxide by mass, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50% of ketones by mass.

The temperature of the catalyst bed in the oxide recycle zone of the reactor was 500 ℃, the catalyst density was 100 kg/m, and the gas velocity was 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst had a carbon content of 0.02% based on the total mass of the catalyst.

The results show an oxide conversion of 98.2 wt% and a combined ethylene and propylene carbon yield of 85.0 wt%.

Comparative example 1

The adopted device comprises a dense-phase section (1) of a reactor, a dilute-phase section (2) of the reactor, a regeneration inclined pipe (5), a cyclone separator (6) and a to-be-regenerated inclined pipe (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the regeneration inclined pipe (5) and the to-be-regenerated inclined pipe (14) are connected with the dense-phase section (1) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor.

Mixed oxide aqueous solution raw materials (8) and methanol raw materials (7) generated by a separation unit in the methanol catalytic conversion process enter a dense-phase section (1) of a reactor to be contacted and reacted with a spent catalyst (15), and generated reaction products (11) enter a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results show an oxide conversion of 50.4 wt% and a combined ethylene and propylene carbon yield of 78.5 wt%.

Comparative example 2

The adopted device comprises a dense phase section (1) of a reactor, a dilute phase section (2) of the reactor, an oxide recycling area (3) of the reactor, a methanol conversion area (4) of the reactor, a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a to-be-regenerated inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 100 degrees, the aperture ratio of the porous region (12) is 40 percent, and the area ratio of the porous region (12) to the non-porous region (13) is 4: 1; the height of the partition (9) accounts for 90 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 500 ℃, the density of the catalyst is 100 kg/cubic meter, and the gas velocity is 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results showed an oxide conversion of 64.5 wt% and a combined ethylene and propylene carbon yield of 80.3 wt%.

Comparative example 3

The adopted device comprises a dense phase section (1) of a reactor, a dilute phase section (2) of the reactor, an oxide recycling area (3) of the reactor, a methanol conversion area (4) of the reactor, a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a to-be-regenerated inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 180 degrees, the aperture ratio of the porous region (12) is 90%, and the area ratio of the porous region (12) to the non-porous region (13) is 0.3: 1; the height of the partition (9) accounts for 50 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 500 ℃, the density of the catalyst is 100 kg/cubic meter, and the gas velocity is 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results showed that the conversion of the oxides was 70.8 wt% and the overall yield of carbon based on ethylene and propylene was 81.1 wt%.

Comparative example 4

The adopted device comprises a dense phase section (1) of a reactor, a dilute phase section (2) of the reactor, an oxide recycling area (3) of the reactor, a methanol conversion area (4) of the reactor, a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a to-be-regenerated inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The baffle (9) is a vertical non-porous plate, and the height of the baffle (9) accounts for 20 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide aqueous solution raw material (8) contains 30% of mixed oxide by mass, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50% of ketones by mass.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 500 ℃, the density of the catalyst is 100 kg/cubic meter, and the gas velocity is 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/m, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results show an oxide conversion of 80.1 wt% and a total yield of ethylene and propylene carbon based 80.7 wt%.

Comparative example 5

The adopted device comprises a dense phase section (1) of a reactor, a dilute phase section (2) of the reactor, an oxide recycling area (3) of the reactor, a methanol conversion area (4) of the reactor, a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a to-be-regenerated inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The baffle (9) is a vertical non-porous plate, and the height of the baffle (9) accounts for 60 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 500 ℃, the density of the catalyst is 100 kg/cubic meter, and the gas velocity is 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results showed 78.2 wt% conversion of the oxygenate and 79.8 wt% total yield of ethylene and propylene carbon based.

Comparative example 6

The adopted device comprises a dense phase section (1) of a reactor, a dilute phase section (2) of the reactor, an oxide recycling area (3) of the reactor, a methanol conversion area (4) of the reactor, a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a to-be-regenerated inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 150 degrees, the aperture ratio of the porous region (12) is 60%, and the area ratio of the porous region (12) to the non-porous region (13) is 2: 1; the height of the partition (9) accounts for 70 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 13: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 500 ℃, the density of the catalyst is 100 kg/cubic meter, and the gas velocity is 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results showed that the conversion of the oxide was 76.5 wt% and the overall yield of ethylene and propylene carbon groups was 80.1 wt%.

Comparative example 7

The adopted device comprises a dense phase section (1) of a reactor, a dilute phase section (2) of the reactor, an oxide recycling area (3) of the reactor, a methanol conversion area (4) of the reactor, a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a to-be-regenerated inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide remixing area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 150 degrees, the aperture ratio of the porous region (12) is 60%, and the area ratio of the porous region (12) to the non-porous region (13) is 2: 1; the height of the partition (9) accounts for 70% of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycling zone (3) of the reactor is 2: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 500 ℃, the density of the catalyst is 100 kg/cubic meter, and the gas velocity is 1.3 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results showed an oxide conversion of 82.4 wt% and a combined ethylene and propylene carbon yield of 81.3 wt%.

[ COMPARATIVE EXAMPLE 8 ]

The adopted device comprises a dense phase section (1) of a reactor, a dilute phase section (2) of the reactor, an oxide recycling area (3) of the reactor, a methanol conversion area (4) of the reactor, a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a to-be-regenerated inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 150 degrees, the aperture ratio of the porous region (12) is 60%, and the area ratio of the porous region (12) to the non-porous region (13) is 2: 1; the height of the partition (9) accounts for 70 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 700 ℃, the density of the catalyst is 60 kg/cubic meter, and the gas velocity is 1.7 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results show an oxide conversion of 95.2 wt% and a total yield of ethylene and propylene carbon based 76.2 wt%.

Comparative example 9

The adopted device comprises a dense phase section (1) of a reactor, a dilute phase section (2) of the reactor, an oxide recycling area (3) of the reactor, a methanol conversion area (4) of the reactor, a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a to-be-regenerated inclined tube (14); wherein: the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor.

Mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10); the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6); the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5).

The partition (9) is composed of a porous region (12) and a non-porous region (13), the porous region (12) is located above the non-porous region (13), the range of an included angle alpha between the porous region (12) and the non-porous region (13) is 150 degrees, the aperture ratio of the porous region (12) is 60%, and the area ratio of the porous region (12) to the non-porous region (13) is 2: 1; the height of the partition (9) accounts for 70 percent of the total height of the dense-phase section (1) of the reactor.

The ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide-recycle zone (3) of the reactor was 7: 1.

The mixed oxide water solution raw material (8) contains 30 percent of mixed oxide by weight, the mixed oxide contains methanol, ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide contains 50 percent of ketones by weight.

The temperature of the catalyst bed in the oxide recycling zone (3) of the reactor is 300 ℃, the density of the catalyst is 200 kg/cubic meter, and the gas velocity is 0.6 m/s.

The temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 490 ℃, the density of the catalyst is 220 kg/cubic meter, and the gas velocity is 1.1 m/s.

The regenerated catalyst (10) had a carbon content of 0.02% based on the total mass of the catalyst.

The results show an oxygenate conversion of 65.7 wt.% and a combined ethylene and propylene carbon yield of 78.5 wt.%.

TABLE 1

TABLE 1 (continuation)

List of comparative examples

Claims (6)

1. A reaction system for oxide recycling in the catalytic conversion process of methanol comprises a dense-phase section (1) of a reactor, a dilute-phase section (2) of the reactor, an oxide recycling area (3) of the reactor, a methanol conversion area (4) of the reactor, a regeneration inclined tube (5), a cyclone separator (6), a partition plate (9) and a to-be-regenerated inclined tube (14); wherein:

the reactor dilute phase section (2) is positioned above the reactor dense phase section (1); the dense-phase section (1) of the reactor consists of a reactor oxide recycling area (3) and a reactor methanol conversion area (4); the regeneration inclined tube (5) is connected with the oxide recycling area (3) of the reactor; the spent inclined tube (14) is connected with the methanol conversion zone (4) of the reactor; the cyclone separator (6) is positioned in the dilute phase section (2) of the reactor; the oxide recycling area (3) of the reactor is connected with the methanol conversion area (4) of the reactor through a partition plate (9), the oxide recycling area (3) of the reactor, the methanol conversion area (4) of the reactor and the partition plate (9) are all positioned in a catalyst bed layer of the dense-phase section (1) of the reactor, and the partition plate (9) is connected with the wall of the reactor;

the partition board (9) consists of a porous area (12) and a non-porous area (13), the porous area (12) is located above the non-porous area (13), the included angle alpha between the porous area (12) and the non-porous area (13) ranges from 120 ︒ to 160 ︒, the aperture ratio of the porous area (12) ranges from 50% to 80%, and the area ratio of the porous area (12) to the non-porous area (13) is (0.5-3): 1; the height of the partition (9) accounts for 50-80% of the total height of the dense-phase section (1) of the reactor; or the baffle (9) is a vertical non-porous plate, and the height of the baffle (9) accounts for 30-50% of the total height of the dense-phase section (1) of the reactor;

the ratio of the volume of the methanol conversion zone (4) of the reactor to the total volume of the oxide recycling zone (3) of the reactor is (3-10): 1.

2. The reaction system for the catalytic conversion of methanol with oxide recycle according to claim 1, wherein the two partitions (9) are arranged in parallel, the middle area of the two partitions (9) is a methanol conversion area (4) of the reactor, and the oxide recycle area of the reactor is divided into an oxide recycle area I (3-1) of the reactor and an oxide recycle area II (3-2) of the reactor.

3. A reaction method for oxide recycling in methanol catalytic conversion process, which adopts any one reaction system of claim 1 or 2, and comprises the following steps:

a) mixed oxide aqueous solution raw materials (8) generated by a separation unit in the methanol catalytic conversion process enter a reactor oxide recycling area (3) to be in contact reaction with a regenerated catalyst (10);

b) the methanol raw material (7) enters a methanol conversion zone (4) of the reactor to be contacted and reacted with a spent catalyst (15), and a generated reaction product (11) enters a subsequent separation system after the catalyst is separated by a cyclone separator (6);

c) the spent catalyst (15) enters a regenerator through a spent inclined tube (14) to burn off carbon deposit to obtain a regenerated catalyst (10), and the regenerated catalyst (10) returns to the oxide recycling area (3) of the reactor through a regenerated inclined tube (5);

the temperature of a catalyst bed layer in the oxide recycling area (3) of the reactor is 480-680 ℃, the density of the catalyst is 70-150 kg/cubic meter, and the gas velocity is 0.8-1.5 m/s.

4. The reaction method for oxide recycling in the catalytic conversion process of methanol according to claim 3, wherein the mixed oxide in the raw material (8) of the mixed oxide aqueous solution comprises 5-70% by weight of mixed oxide, the mixed oxide comprises methanol and at least one of ethanol, propanol, butanol, formaldehyde, acetaldehyde, propionaldehyde, butyraldehyde, acetone, butanone, formic acid, acetic acid and propionic acid, and the mixed oxide comprises 30-80% by weight of ketones.

5. The reaction method for oxide recycling in the catalytic conversion process of methanol as claimed in claim 3, wherein the temperature of the catalyst bed in the methanol conversion zone (4) of the reactor is 450-550 ℃, the density of the catalyst is 200-500 kg/m, and the gas velocity is 0.5-1.5 m/s.

6. The reaction process for the catalytic conversion of methanol with oxide recycling according to claim 3, characterized in that the regenerated catalyst (10) has a carbon content of less than 0.1% by mass of the total mass of the catalyst.

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