CN113842842B - Device and method for preparing olefin by catalytic conversion of methanol - Google Patents
Device and method for preparing olefin by catalytic conversion of methanol Download PDFInfo
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- CN113842842B CN113842842B CN202010599369.4A CN202010599369A CN113842842B CN 113842842 B CN113842842 B CN 113842842B CN 202010599369 A CN202010599369 A CN 202010599369A CN 113842842 B CN113842842 B CN 113842842B
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Abstract
The invention discloses a device for preparing olefin by catalytic conversion of methanol, which comprises: a fast fluidized bed reactor (6); a secondary dense bed (8) which is connected with the fast fluidized bed reactor (6) through a circulating inclined pipe (1); an external heat collector (7) which is connected with the fast fluidized bed reactor (6) through an external inclined tube (2) and is connected with the secondary dense bed (8); a regenerator (10) connected to the fast fluidized bed reactor (6) through a regeneration chute (3); the outlet end of the circulating inclined pipe (1) is provided with a circulating inclined pipe horizontal section, and a circulating inclined pipe feeding pipe descending section (4-1) is arranged behind the circulating inclined pipe horizontal section; the outlet end of the external inclined tube (2) is provided with an external inclined tube horizontal section, and an external inclined tube feeding pipe descending section (4-2) is arranged behind the external inclined tube horizontal section. The invention also discloses a method for preparing olefin by catalytic conversion of methanol. The invention better solves the problems in the prior art and can be applied industrially.
Description
Technical Field
The invention relates to a device for preparing olefin by catalytic conversion of methanol and a method for preparing olefin by catalytic conversion of methanol by using the device.
Background
Ethylene and propylene are important basic chemical raw materials, and the industrial demand thereof is increasing. Because of limited petroleum resources and high price, the cost of producing ethylene and propylene by the traditional petroleum route is continuously increased. Methanol is used as a raw material, and SAPO-34 and ZSM-5 catalysts are adopted to react to obtain ethylene, propylene, aromatic hydrocarbon and gasoline products. The process for preparing methanol from coal or natural gas is mature, and the methanol is cheap due to rich coal resources in China. The catalytic conversion of methanol to ethylene, propylene, aromatic hydrocarbon and gasoline is receiving more and more attention, and related technical researches and patents are very numerous.
CN103288570B discloses a device and a method for preparing olefin from methanol, wherein a radial baffle is arranged between a feed distribution plate and a raw material inlet, and a regenerator main air distributor, a spent catalyst external branch distributor, a regenerator grid and other members are arranged on a reactor to promote the mixing of catalysts.
CN105214572B discloses a reaction-regeneration device and a reaction method for preparing olefin from methanol, wherein a baffle is arranged in a regeneration inclined tube, and a supplementary gas line is arranged in an ascending tube of a fast fluidized bed reactor to supplement and convey gas from bottom to top.
CN105457569B discloses a double-regenerator reaction device and a reaction method for preparing low-carbon olefin from methanol, wherein the device is provided with two regeneration devices, namely a fast fluidized bed regenerator and a turbulent bed regenerator.
Disclosure of Invention
The invention aims to provide a device for preparing olefin by catalytic conversion of methanol and a method for preparing olefin by catalytic conversion of methanol by using the device, aiming at the problem of uneven distribution of carbon deposition of a regenerated catalyst in an MTO device in the prior art. The invention better solves the problems in the prior art and can be applied industrially.
According to one aspect of the present invention, there is provided an apparatus for producing olefins by catalytic conversion of methanol, comprising:
a fast fluidized bed reactor (6);
a secondary dense bed (8) which is connected with the fast fluidized bed reactor (6) through a circulating inclined pipe (1);
an external heat collector (7) which is connected with the fast fluidized bed reactor (6) through an external inclined tube (2) and is connected with the second dense bed (8);
a regenerator (10) connected to the fast fluidized bed reactor (6) through a regeneration chute (3);
according to a preferred embodiment of the invention, the outlet end of the circulation chute (1) is provided with a circulation chute horizontal section extending through the side wall of the fast fluidized bed reactor (6) to the interior of the fast fluidized bed reactor (6); a descending section (4-1) of the circulating inclined tube feeding tube is arranged behind the horizontal section of the circulating inclined tube, and preferably, the descending section (4-1) of the circulating inclined tube feeding tube forms an included angle of 10-30 degrees with the horizontal direction;
according to a preferred embodiment of the invention, the outlet end of the outer chute (2) is provided with an outer chute horizontal section which extends through the side wall of the fast fluidized bed reactor (6) to the interior of the fast fluidized bed reactor (6); an outer inclined tube feeding tube descending section (4-2) is arranged behind the horizontal section of the outer inclined tube, and preferably, the included angle between the outer inclined tube feeding tube descending section (4-2) and the horizontal direction is 10-30 degrees.
According to some embodiments of the invention, the outlets of the descending sections (4-1, 4-2) of the circulating pipe chute feed pipes are on the same horizontal plane, and the outlets are in opposite directions.
The outlets of the descending section (4-1) of the circulating inclined tube feeding pipe and the descending section (4-2) of the external inclined tube feeding pipe are arranged on the same plane and opposite in direction, materials discharged from the descending section (4-1) of the circulating inclined tube feeding pipe and the descending section (4-2) of the external inclined tube feeding pipe can be fully mixed, and a plurality of strands of catalysts with different temperatures and carbon deposition amounts can be fully mixed to ensure the stability and high efficiency of the reaction for preparing olefin through catalytic conversion of methanol.
According to the preferred embodiment of the invention, the descending section (4-1) of the circulation inclined pipe feeding pipe is provided with a guide plate.
According to the preferred embodiment of the invention, the descending section (4-2) of the external inclined pipe feeding pipe is provided with a guide plate.
The arrangement of the guide plate has a further promotion effect on the mixing of materials, the disturbance of the catalyst in the fast fluidized bed reactor (6) can be enhanced, and the mixing of the catalyst can be further promoted.
According to some embodiments of the invention, the device comprises 1 circulation inclined pipe (1), the included angle between the projections of the circulation inclined pipe (1) and the outer inclined pipe (2) on the horizontal plane is alpha, and the alpha is more than 30 degrees and less than or equal to 180 degrees.
According to the preferred embodiment of the invention, the outlet end of the circulation inclined tube (1) is provided with 1 descending section (4-1) of the feeding tube of the circulation inclined tube, and the included angle between the extension line of the projection of the circulation inclined tube (1) on the horizontal plane and the projection of the descending section (4-1) of the feeding tube of the circulation inclined tube on the horizontal plane is beta; β ═ 180 ° - α)/2.
According to the preferred embodiment of the invention, the outlet end of the external inclined tube (2) is provided with 1 external inclined tube feeding tube descending section (4-2), and the included angle between the extension line of the projection of the external inclined tube (2) on the horizontal plane and the projection of the external inclined tube feeding tube descending section (4-2) on the horizontal plane is beta; β ═ 180 ° - α)/2.
Through the arrangement, the outlet directions of the descending section (4-1) of the circulating inclined tube feeding pipe and the descending section (4-2) of the externally-taken inclined tube feeding pipe are opposite, so that the materials are conveniently mixed, and the materials can be fully mixed in the first time after coming out.
According to some embodiments of the invention, the device comprises n circulation pipes (1), n is greater than or equal to 2, preferably n is 2-10; the adjacent circulating inclined pipes (1) or the adjacent circulating inclined pipes (1) and the projections of the outer inclined pipes (2) on the horizontal plane form an included angle alpha', which is 360 degrees/n + 1.
When a plurality of circulating inclined pipes exist, only one regenerating inclined pipe is connected with the horizontal section of one circulating inclined pipe.
According to the preferred embodiment of the invention, 2 descending sections (4-1) of the feeding pipe of the circulating inclined pipe are arranged at the outlet end of each circulating inclined pipe (1), and the 2 descending sections (4-1) of the feeding pipe of the circulating inclined pipe at the outlet end of each circulating inclined pipe (1) are symmetrical according to the extension line of the circulating inclined pipe (1); namely, each circulation inclined pipe (1) is connected with the descending sections (4-1) of 2 circulation inclined pipe feeding pipes connected with the circulation inclined pipe (1) in a Y shape. An included angle between the extension line of the projection of each circulation inclined pipe (1) on the horizontal plane and the projection of the descending section (4-1) of the circulation inclined pipe feeding pipe at the outlet end of the circulation inclined pipe on the horizontal plane is beta'; β ═ 180 ° - α')/2.
According to the preferred embodiment of the invention, the outlet end of the external inclined tube (2) is provided with 2 external inclined tube feeding tube descending sections (4-2), and the 2 external inclined tube feeding tube descending sections (4-2) at the outlet end of the external inclined tube (2) are symmetrical according to the extension line of the external inclined tube (2); namely, the external inclined tube (2) is connected with the descending sections (4-2) of the 2 external inclined tube feeding pipes connected with the external inclined tube in a Y shape. An included angle between an extension line of the projection of the external inclined tube (2) on the horizontal plane and the projection of a descending section (4-2) of the external inclined tube feeding tube at the outlet end of the external inclined tube on the horizontal plane is beta'; β ═ 180 ° - α')/2.
Through the arrangement, the outlet directions of the descending section (4-1) of the at least one circulating inclined tube feeding pipe and the descending section (4-2) of the external inclined tube feeding pipe are opposite, so that the materials can be conveniently mixed, and the materials can be fully mixed in the first time after coming out.
According to some embodiments of the invention, the regenerator (10) includes a dense phase section and a lean phase section.
According to a preferred embodiment of the invention, the dense phase section is below the lean phase section.
According to a preferred embodiment of the invention, the lean phase section of the regenerator is connected to the fast fluidized bed reactor (6) via a regeneration chute (3) and the dense phase section of the regenerator is connected to the dense bed (8) via a spent chute (9).
According to a preferred embodiment of the invention, the outlet end of the regeneration chute (3) is provided with a regeneration chute horizontal section extending through the circulation chute horizontal section to the interior of the circulation chute horizontal section.
According to a preferred embodiment of the invention, the horizontal section of the regeneration chute and the horizontal section of the circulation chute are arranged coaxially, the diameter of the regeneration chute (3) being smaller than the diameter of the circulation chute (1).
According to the preferred embodiment of the invention, the upper outlet of the fast fluidized bed reactor (6) is connected with the lower inlet of the secondary dense bed (8), and the connection position is positioned in the secondary dense bed (8).
According to some embodiments of the invention, a gas phase feed distributor (5) is disposed within the fast fluidized bed reactor (6), the gas phase feed distributor (5) being located below the circulating chute feed pipe drop section (4-1) and the external withdrawal chute feed pipe drop section (4-2).
According to a preferred embodiment of the invention, the top of the two dense beds is provided with a product gas outlet (12) for discharging product gas.
According to a preferred embodiment of the invention, the top of the regenerator (10) is provided with a flue gas outlet (13) for discharging flue gas in the regenerator (10); the bottom of the regenerator (10) is provided with a regeneration medium inlet (11) for introducing a regeneration medium.
In another aspect, the present invention provides a method for preparing olefin by catalytic conversion of methanol, which uses the apparatus of the first aspect, and includes the following steps:
(a) methanol enters a fast fluidized bed reactor (6) to be fluidized and react with a catalyst, and the catalyst enters a secondary dense bed (8) along with gas phase material flow;
(b) the gas phase material flow is separated in a double dense bed (8) to obtain product gas and discharged, and the catalyst is divided into three parts; the first strand is used as a circulating spent agent and returns to the fast fluidized bed reactor (6) through the circulating inclined pipe (1); the second part as an external spent agent returns to the fast fluidized bed reactor (6) through an external heat collector (7) and an external inclined tube (2); the third stream enters a regenerator (10) and returns to the fast fluidized bed reactor (6) as a regenerant through a regeneration inclined tube (3) after regeneration.
According to some embodiments of the invention, in step (a), the gas phase material methanol enters the fast fluidized bed reactor (6) through the gas phase feed distributor (5), and is fluidized and reacted with the catalyst, and the catalyst enters the dense bed (8) along with the gas phase material flow.
According to a preferred embodiment of the invention, the gas phase stream comprises unreacted methanol and products.
According to a preferred embodiment of the invention, in step (b), the product gas is separated by separation means such as a cyclone.
According to some embodiments of the invention, in step (b), the catalyst is divided into three streams, the first stream being returned to the fast fluidized bed reactor (6) as recycle spent via the recycle chute (1) via the recycle chute feed pipe drop (4-1); the second strand as an external spent agent returns to the fast fluidized bed reactor (6) through an external heat collector (7) and an external inclined tube (2) via an external inclined tube feeding pipe descending section (4-2); and the third strand enters a regenerator (10) through a to-be-regenerated inclined tube (9), is used as a regenerant after regeneration, enters the horizontal section of the circulating inclined tube (1) through a regeneration inclined tube (3) to be mixed with the circulating to-be-regenerated agent, is discharged through a descending section (4-1) of a feeding tube of the circulating inclined tube after being mixed with the circulating to-be-regenerated agent, and is then secondarily mixed with an externally-taken to-be-regenerated agent.
According to the preferred embodiment of the present invention, the uniformly mixed catalyst enters the two-dense bed and then falls down due to gravity and flows out randomly from each outlet, and the catalyst is divided into three streams.
According to the preferred embodiment of the invention, the gas phase material methanol further mixes and reacts with the three catalyst strands (the regenerant, the circulating spent catalyst and the external spent catalyst) during the upward conveying process along the axial direction, and the guide plates arranged on the descending section (4-1) of the circulating inclined tube feeding pipe and the descending section (4-2) of the external inclined tube feeding pipe have the function of further promoting the mixing of the three catalyst strands.
According to the preferred embodiment of the invention, when the number of the circulation inclined pipes (1) is more than 1, the multiple catalysts are secondarily mixed two by two at the outlet of each descending section (4-1) of the circulation inclined pipe feeding pipe and/or the descending section (4-2) of the external inclined pipe feeding pipe, and the mixed multiple catalyst materials are further mixed for the third time in the process of ascending along with the gas-phase methanol feeding.
According to the preferred embodiment of the present invention, the temperature in the fast fluidized bed reactor (6) is 400-500 ℃, preferably 430-500 ℃; a pressure of 0.05 to 0.4MPaG, preferably 0.1 to 0.4 MPaG; the space velocity is 2-20h -1 Preferably 5-20h -1 。
According to a preferred embodiment of the invention, the temperature of the circulating spent catalyst is 430-500 ℃, preferably 440-500 ℃; and/or the temperature of the external spent reagent is 250-430 ℃, preferably 250-420 ℃; and/or the temperature of the regenerant is 500-700 ℃, preferably 510-690 ℃; and/or the feed flux of the circulating spent agent is 20-300kg/m 2 s, preferably 40 to 280kg/m 2 s; and/or the feeding flux of the external spent agent is 20-300kg/m 2 s, preferably 40 to 280kg/m 2 s; and/or the feed flux of the regenerant is from 20 to 300kg/m 2 s, preferably 40 to 280kg/m 2 s; and/or the recycling amount of the regenerant accounts for 1/30-1/10, preferably 1/25-1/15 of the total recycling amount.
The invention has the advantages and beneficial technical effects as follows:
the invention makes the regenerant, the circulating spent regenerant and the external spent regenerant fully mixed by the structure of the regenerating inclined tube, the optimization of the position between the regenerating inclined tube and the circulating inclined tube and the specific layout relationship between the circulating inclined tube, the external heat-taking tube and the descending section of the feeding tube. By mixing a plurality of strands of catalysts with different temperatures and carbon deposition amounts, the properties of the mixed catalysts are more stable and uniform, and the stability and the high efficiency of the reaction for preparing the olefin by the catalytic conversion of the methanol are facilitated.
Drawings
FIG. 1 is a schematic diagram of an apparatus for producing olefins by catalytic conversion of methanol according to the present invention:
FIG. 2 is an enlarged view of a part of the structure of a regeneration inclined tube and a circulation inclined tube;
FIG. 3 is a top view of the placement of the circulation chute and the external pick-up chute for 1 circulation chute;
FIG. 4 is a top view of the placement of the circulation chute and the external pick-up chute for the 2 circulation chutes;
FIG. 5 is a top view of the orientation of the circulation chute and external ramps for the case of 3 circulation chutes.
FIG. 6 is a plan view showing the arrangement orientation of the circulation, external-take and regeneration ramps of comparative example 2.
In the figure, 1 is a circulating inclined pipe; 2 is an external inclined tube; 3 is a regeneration inclined tube; 4-1 is a descending section of the circular inclined tube feeding tube; 4-2 is a descending section of the external inclined tube feeding tube; 5 is a gas phase feeding distributor; 6 is a fast fluidized bed reactor; 7 is an external heat collector; 8 is a dense bed; 9 is a to-be-grown inclined tube; 10 is a regenerator; 11 is a regeneration medium inlet; 12 is a product gas outlet; 13 is a smoke outlet;
Detailed Description
The invention is further illustrated by the following figures and examples, but is not limited to these examples.
[ example 1 ] A method for producing a polycarbonate
The circulating inclined tube (1) is connected with the two dense beds (8) and the fast fluidized bed reactor (6), the outlet end of the circulating inclined tube (1) is provided with a circulating inclined tube horizontal section, and the circulating inclined tube horizontal section penetrates through the side wall of the fast fluidized bed reactor (6) and extends into the fast fluidized bed reactor (6); a descending section (4-1) of the circulating inclined tube feeding tube is arranged behind the horizontal section of the circulating inclined tube, and the angle between the descending section (4-1) of the circulating inclined tube feeding tube and the horizontal direction is 30 degrees.
The outer inclined tube (2) is connected with an outer heater (7) and the fast fluidized bed reactor (6), the outlet end of the outer inclined tube (2) is provided with an outer inclined tube horizontal section, and the outer inclined tube horizontal section penetrates through the side wall of the fast fluidized bed reactor (6) and extends into the fast fluidized bed reactor (6); an outer inclined tube feeding pipe descending section (4-2) is arranged behind the horizontal section of the outer inclined tube, and the included angle between the outer inclined tube feeding pipe descending section (4-2) and the horizontal direction is 30 degrees.
The outlets of the descending section (4-1) of the circulating inclined tube feeding tube and the descending section (4-2) of the external inclined tube feeding tube are on the same horizontal plane, and the outlet directions are opposite. The device in the embodiment comprises 1 circulating inclined tube (1), and the included angle alpha between the projections of the circulating inclined tube (1) and the external inclined tube (2) on the horizontal plane is 180 degrees.
The regeneration inclined tube (3) is connected with the phase thinning section of the regenerator (10) and the fast fluidized bed reactor (6), the outlet end of the regeneration inclined tube (3) is provided with a regeneration inclined tube horizontal section, and the regeneration inclined tube horizontal section penetrates through the circulation inclined tube horizontal section and extends to the interior of the circulation inclined tube horizontal section; the horizontal sections of the regeneration inclined tube and the horizontal section of the circulation inclined tube are coaxially arranged, and the diameter of the regeneration inclined tube is smaller than that of the circulation inclined tube (shown in figure 2).
The gas phase feeding distributor (5) is arranged inside the fast fluidized bed reactor (6) and is positioned below the descending section (4-1) of the circulating inclined tube feeding pipe and the descending section (4-2) of the external inclined tube feeding pipe.
The external heat collector (7) is connected with the fast fluidized bed reactor (6) through an external inclined tube (2) and is connected with the two dense beds (8) through a pipeline.
The lower inlet of the second dense bed (8) is connected with the upper outlet of the fast fluidized bed reactor (6), the joint is positioned in the second dense bed (8), and the top of the second dense bed is provided with a product gas outlet (12).
The regenerator (10) includes a dense phase section and a lean phase section, the dense phase section being below the lean phase section; the phase thinning section of the regenerator (10) is connected with the fast fluidized bed reactor (6) through a regeneration inclined pipe (3), and the dense phase section is connected with a dense bed (8) through a to-be-generated inclined pipe (9); the top of the regenerator (10) is provided with a flue gas outlet (13), and the bottom is provided with a regeneration medium inlet (11).
[ example 2 ]
Basically the same as the embodiment 1, except that the device in this embodiment comprises 1 circulation inclined tube (1), the included angle alpha between the projections of the circulation inclined tube (1) and the external inclined tube (2) on the horizontal plane is 120 degrees, the included angle beta between the extension line of the projection of the circulation inclined tube (1) on the horizontal plane and the projection of the descending section (4-1) of the feeding tube of the circulation inclined tube on the horizontal plane and the included angle beta between the extension line of the projection of the external inclined tube (2) on the horizontal plane and the projection of the descending section (4-2) of the feeding tube of the external inclined tube on the horizontal plane are 30 degrees (as shown in fig. 3).
[ example 3 ]
The device is basically the same as the device in the embodiment 1, except that the device in the embodiment comprises 2 circulating inclined pipes (1), the included angle between the projections of the circulating inclined pipes (1) and the external inclined pipes (2) on the horizontal plane and the included angle alpha' between the projections of the two circulating inclined pipes (1) on the horizontal plane are 120 degrees. The outlet end of each circulation inclined pipe (1) is provided with 2 circulation inclined pipe feeding pipe descending sections (4-1), and the 2 circulation inclined pipe feeding pipe descending sections (4-1) at the outlet end of each circulation inclined pipe (1) are symmetrical along the extension line of the circulation inclined pipe (1); namely, the descending sections (4-1) of the 2 circulating inclined tube feeding pipes connected with the circulating inclined tube (1) are connected in a Y shape. An included angle beta' between the extension line of the projection of each circulation inclined tube (1) on the horizontal plane and the projection of one circulation inclined tube feeding tube descending section (4-1) at the outlet end of the circulation inclined tube on the horizontal plane is 30 degrees, and an included angle beta between 2 circulation inclined tube feeding tube descending sections (4-1) at the outlet end of the same circulation inclined tube (1) is 60 degrees. The outlet end of the external inclined tube (2) is provided with 2 external inclined tube feeding tube descending sections (4-2), and the 2 external inclined tube feeding tube descending sections (4-2) at the outlet end of the external inclined tube (2) are symmetrical according to the extension line of the external inclined tube (2); namely, the external inclined tube (2) is connected with the descending sections (4-2) of the 2 external inclined tube feeding pipes connected with the external inclined tube in a Y shape. An included angle beta' between the extension line of the projection of the external inclined tube (2) on the horizontal plane and the projection of the descending section (4-2) of the external inclined tube feeding tube at the outlet end of the external inclined tube on the horizontal plane is 30 degrees, and an included angle beta between the descending sections (4-2) of the 2 external inclined tube feeding tubes at the outlet end of the external inclined tube (2) is 60 degrees (as shown in figure 4).
[ example 4 ] A method for producing a polycarbonate
Basically the same as the embodiment 1, except that the device in the embodiment comprises 3 circulation inclined pipes (1), the included angle between the projections of the circulation inclined pipes (1) and the external inclined pipes (2) on the horizontal plane and the included angle alpha' between the projections of two adjacent circulation inclined pipes (1) on the horizontal plane are 90 degrees. The outlet end of each circulation inclined pipe (1) is provided with 2 circulation inclined pipe feeding pipe descending sections (4-1), and the 2 circulation inclined pipe feeding pipe descending sections (4-1) at the outlet end of each circulation inclined pipe (1) are symmetrical along the extension line of the circulation inclined pipe (1); namely, the descending sections (4-1) of the 2 circulating inclined tube feeding pipes connected with the circulating inclined tube (1) are connected in a Y shape. The included angle beta' between the extension line of the projection of each circulating inclined tube (1) on the horizontal plane and the projection of the descending section (4-1) of one circulating inclined tube feeding tube at the outlet end of the circulating inclined tube on the horizontal plane is 45 degrees, and the included angle between the descending sections (4-1) of 2 circulating inclined tube feeding tubes at the outlet end of the same circulating inclined tube (1) is 90 degrees. 2 outer inclined pipe feeding pipe descending sections (4-2) are arranged at the outlet end of the outer inclined pipe (2), and the 2 outer inclined pipe feeding pipe descending sections (4-2) at the outlet end of the outer inclined pipe (2) are symmetrical according to the extension line of the outer inclined pipe (2); namely, the outer inclined tube (2) is connected with the descending sections (4-2) of the 2 outer inclined tube feeding tubes connected with the outer inclined tube in a Y shape. An included angle beta' between the extension line of the projection of the external inclined tube (2) on the horizontal plane and the projection of the descending section (4-2) of the external inclined tube feeding tube at the outlet end of the external inclined tube on the horizontal plane is 45 degrees, and an included angle beta between the descending sections (4-2) of the 2 external inclined tube feeding tubes at the outlet end of the external inclined tube (2) is 90 degrees (as shown in figure 5).
[ example 5 ]
The reaction for producing olefins by catalytic conversion of methanol using the apparatus of example 1 comprises:
the gas phase material methanol enters a fast fluidized bed reactor (6) through a gas phase feeding distributor (5) to be fluidized and react with the catalyst, and the catalyst enters a dense bed (8) along with gas phase material flow.
The gas phase material flow is separated in a secondary dense bed (8) to obtain product gas and discharged, the catalyst is divided into three parts, and the first part serving as a circulating spent catalyst is returned to the fast fluidized bed reactor (6) through a descending section (4-1) of a circulating inclined tube feeding pipe through a circulating inclined tube (1); the second strand as an external spent agent returns to the fast fluidized bed reactor (6) through an external heat collector (7) and an external inclined tube (2) via an external inclined tube feeding pipe descending section (4-2); and the third strand enters a regenerator (10) through a to-be-regenerated inclined tube (9), is used as a regenerant after regeneration, enters the horizontal section of the circulating inclined tube (1) through a regeneration inclined tube (3) to be mixed with the circulating to-be-regenerated agent, is discharged through a descending section (4-1) of a feeding tube of the circulating inclined tube after being mixed with the circulating to-be-regenerated agent, and is then secondarily mixed with an externally-taken to-be-regenerated agent.
Wherein the temperature of the circulating spent catalyst is 450 ℃, the temperature of the externally-taken spent catalyst is 300 ℃, the temperature of the regenerant is 600 ℃, and the feeding flux of the circulating spent catalyst is 150kg/m 2 s, the feeding flux of the external spent agent is 150kg/m 2 s, regenerant feed flux of 250kg/m 2 s, the regenerant recycle amount is 1/20 of the total recycle amount. The temperature in the fast fluidized bed reactor (6) is 450 ℃, the pressure is 0.2MPaG, and the space velocity is 10h -1 。
The conversion of methanol was 99.2%, and the total yield of ethylene and propylene was 85.9%.
[ example 6 ]
The reaction for producing olefins by catalytic conversion of methanol using the apparatus of example 2 comprises:
the gas phase material methanol enters a fast fluidized bed reactor (6) through a gas phase feeding distributor (5) to be fluidized and react with the catalyst, and the catalyst enters a dense bed (8) along with gas phase material flow.
The gas phase material flow is separated in a secondary dense bed (8) to obtain product gas and discharged, the catalyst is divided into three parts, and the first part serving as a circulating spent catalyst is returned to the fast fluidized bed reactor (6) through a descending section (4-1) of a circulating inclined tube feeding pipe through a circulating inclined tube (1); the second strand as an external spent agent returns to the fast fluidized bed reactor (6) through an external heat collector (7) and an external inclined tube (2) via an external inclined tube feeding pipe descending section (4-2); and the third strand enters a regenerator (10) through a to-be-regenerated inclined tube (9), is used as a regenerant after regeneration, enters the horizontal section of the circulating inclined tube (1) through a regeneration inclined tube (3) to be mixed with the circulating to-be-regenerated agent, is discharged through a descending section (4-1) of a feeding tube of the circulating inclined tube after being mixed with the circulating to-be-regenerated agent, and is then secondarily mixed with an externally-taken to-be-regenerated agent.
Wherein the temperature of the circulating spent catalyst is 450 ℃, the temperature of the external spent catalyst is 300 ℃, the temperature of the regenerant is 600 ℃, and the feeding flux of the circulating spent catalyst is 150kg/m 2 s, the feeding flux of the external spent agent is 150kg/m 2 s, regenerant feed flux of 250kg/m 2 s, the regenerant recycle amount was 1/20 of the total recycle amount. The temperature in the fast fluidized bed reactor (6) is 450 ℃, the pressure is 0.2MPaG, and the space velocity is 10h -1 。
The conversion of methanol was 99.6%, and the total yield of ethylene and propylene was 84.3%.
[ example 7 ]
The reaction for producing olefins by catalytic conversion of methanol using the apparatus of example 3 comprises:
the gas phase material methanol enters a fast fluidized bed reactor (6) through a gas phase feeding distributor (5) to be fluidized and react with the catalyst, and the catalyst enters a dense bed (8) along with gas phase material flow.
The gas phase material flow is separated in a secondary dense bed (8) to obtain product gas and discharged, the catalyst is divided into three parts, and the first part serving as a circulating spent catalyst is returned to the fast fluidized bed reactor (6) through 2 circulating inclined pipes (1) via a descending section (4-1) of a circulating inclined pipe feeding pipe; the second strand as an external spent agent returns to the fast fluidized bed reactor (6) through an external heat collector (7) and an external inclined tube (2) via an external inclined tube feeding pipe descending section (4-2); and the third strand enters a regenerator (10) through a to-be-regenerated inclined pipe (9), is used as a regenerant after regeneration, enters a horizontal section of a circulating inclined pipe (1) through a regenerating inclined pipe (3) to be mixed with the circulating to-be-regenerated agent, is discharged through a descending section (4-1) of a circulating inclined pipe feeding pipe after being mixed with the circulating to-be-regenerated agent, and is then secondarily mixed with an externally-taken to-be-regenerated agent. The multiple catalysts are secondarily mixed at the outlet of the descending section (4-2) of the external inclined tube feeding pipe and/or the descending section (4-1) of the circulating inclined tube feeding pipe, and the mixed multiple catalysts are further thirdly mixed in the process of ascending along with the feeding of the gas-phase methanol.
Wherein the temperature of the circulating spent catalyst is 450 ℃, the temperature of the external spent catalyst is 300 ℃, the temperature of the regenerant is 600 ℃, and the feeding flux of the circulating spent catalyst is 150kg/m 2 s, the feeding flux of the external spent agent is 150kg/m 2 s, regenerant feed flux of 250kg/m 2 s, the regenerant recycle amount is 1/20 of the total recycle amount. The temperature in the fast fluidized bed reactor (6) is 450 ℃, the pressure is 0.2MPaG, and the space velocity is 10h -1 。
The conversion of methanol was 99.5%, and the total yield of ethylene and propylene was 86.3%.
[ example 8 ]
The reaction for producing olefins by catalytic conversion of methanol using the apparatus of example 4 comprises:
the gas phase material methanol enters a fast fluidized bed reactor (6) through a gas phase feeding distributor (5) to be fluidized and react with the catalyst, and the catalyst enters a dense bed (8) along with gas phase material flow.
The gas phase material flow is separated in a secondary dense bed (8) to obtain product gas and discharged, the catalyst is divided into three parts, and the first part serving as a circulating spent catalyst is returned to the fast fluidized bed reactor (6) through a descending section (4-1) of a circulating inclined pipe feeding pipe through 3 circulating inclined pipes (1); the second strand as an external spent agent returns to the fast fluidized bed reactor (6) through an external heat collector (7) and an external inclined tube (2) via an external inclined tube feeding pipe descending section (4-2); and the third strand enters a regenerator (10) through a to-be-regenerated inclined pipe (9), is used as a regenerant after regeneration, enters a horizontal section of a circulating inclined pipe (1) adjacent to the external inclined pipe (2) through a regeneration inclined pipe (3) to be mixed with the circulating to-be-regenerated agent, is discharged through a descending section (4-1) of a circulating inclined pipe feeding pipe after being mixed with the circulating to-be-regenerated agent, and is then secondarily mixed with the external to-be-regenerated agent. The multiple catalysts are secondarily mixed at the outlet of the descending section (4-2) of the external inclined tube feeding pipe and/or the descending section (4-1) of the circulating inclined tube feeding pipe, and the mixed multiple catalysts are further thirdly mixed in the process of ascending along with the feeding of the gas-phase methanol.
Wherein the temperature of the circulating spent catalyst is 450 ℃, the temperature of the externally-taken spent catalyst is 300 ℃, the temperature of the regenerant is 600 ℃, and the feeding flux of the circulating spent catalyst is 150kg/m 2 s, the feeding flux of the external spent agent is 150kg/m 2 s, regenerant feed flux of 250kg/m 2 s, the regenerant recycle amount is 1/20 of the total recycle amount. The temperature in the fast fluidized bed reactor (6) is 450 ℃, the pressure is 0.2MPaG, and the space velocity is 10h -1 。
The conversion of methanol was 99.9%, and the total yield of ethylene and propylene was 87.5%.
Comparative example 1
The same as the example 5, except that the device is not provided with a descending section (4-1) of the feeding pipe of the circulating inclined pipe (1) at the outlet and is not provided with a descending section (4-2) of the feeding pipe of the external inclined pipe (2) at the outlet.
The conversion of methanol was 99.0% and the total yield of ethylene and propylene was 83.2%.
Comparative example 2
The same as in example 5, except that the regeneration chute (3) in the apparatus did not extend into the circulation chute (1) and was passed directly into the barrel of the fast-fluidized-bed reactor (6) (as shown in FIG. 6).
The methanol conversion was 99.4%, and the total yield of ethylene and propylene was 82.3%.
Comparative example 3
The device is the same as the comparative example 2, except that the outlet of the circulating inclined tube (1) in the device is not provided with a descending section (4-1) of the circulating inclined tube feeding tube, and the outlet of the external inclined tube (2) is not provided with a descending section (4-2) of the external inclined tube feeding tube.
The conversion of methanol was 99.2%, and the total yield of ethylene and propylene was 81.8%.
Any numerical value mentioned in this specification, if there is only a two unit interval between any lowest value and any highest value, includes all values from the lowest value to the highest value incremented by one unit at a time. For example, if it is stated that the amount of a component, or a value of a process variable such as temperature, pressure, time, etc., is 50 to 90, it is meant in this specification that values of 51 to 89, 52 to 88 … …, and 69 to 71, and 70 to 71, etc., are specifically enumerated. For non-integer values, units of 0.1, 0.01, 0.001, or 0.0001 may be considered as appropriate. These are only some specifically named examples. In a similar manner, all possible combinations of numerical values between the lowest value and the highest value enumerated are to be considered to be disclosed in this application.
It should be noted that the above-mentioned embodiments are only for explaining the present invention, and do not constitute any limitation to the present invention. The present invention has been described with reference to exemplary embodiments, but the words which have been used herein are words of description and illustration, rather than words of limitation. The invention can be modified, as prescribed, within the scope of the claims and without departing from the scope and spirit of the invention. Although the invention has been described herein with reference to particular means, materials and embodiments, the invention is not intended to be limited to the particulars disclosed herein, but rather extends to all other methods and applications having the same functionality.
Claims (14)
1. An apparatus for producing olefins by catalytic conversion of methanol, comprising:
a fast fluidized bed reactor (6);
a secondary dense bed (8) which is connected with the fast fluidized bed reactor (6) through a circulating inclined pipe (1);
an external heat collector (7) which is connected with the fast fluidized bed reactor (6) through an external inclined tube (2) and is connected with the secondary dense bed (8);
a regenerator (10) connected to the fast fluidized bed reactor (6) by a regeneration chute (3);
the outlet end of the inclined circulating pipe (1) is provided with a horizontal circulating pipe section which penetrates through the side wall of the fast fluidized bed reactor (6) and extends into the fast fluidized bed reactor (6); a descending section (4-1) of the circulating inclined pipe feeding pipe is arranged behind the horizontal section of the circulating inclined pipe, and the angle between the descending section (4-1) of the circulating inclined pipe feeding pipe and the horizontal direction is 10-30 degrees;
the outlet end of the outer inclined tube (2) is provided with an outer inclined tube horizontal section which penetrates through the side wall of the fast fluidized bed reactor (6) and extends into the fast fluidized bed reactor (6); an outer inclined tube feeding tube descending section (4-2) is arranged behind the horizontal section of the outer inclined tube, and the included angle between the outer inclined tube feeding tube descending section (4-2) and the horizontal direction is 10-30 degrees;
outlets of the descending section (4-1) of the circulating inclined tube feeding tube and the descending section (4-2) of the external inclined tube feeding tube are on the same horizontal plane, and the directions of the outlets are opposite;
and the outlet end of the regeneration inclined tube (3) is provided with a regeneration inclined tube horizontal section, and the regeneration inclined tube horizontal section penetrates through the circulation inclined tube horizontal section and extends to the inside of the circulation inclined tube horizontal section.
2. The device according to claim 1, characterized in that the descending section (4-1) of the circulating inclined tube feeding pipe is provided with a flow guide plate; and/or a guide plate is arranged on the descending section (4-2) of the external inclined pipe feeding pipe.
3. The device according to any one of claims 1-2, characterized in that the device comprises 1 circulation chute (1), and the included angle between the projections of the circulation chute (1) and the external extraction chute (2) on the horizontal plane is alpha, 30 ° < alpha ≦ 180 °.
4. The apparatus according to claim 3, characterized in that the outlet end of the circulation chute (1) is provided with 1 circulation chute feed pipe drop (4-1), and the angle between the extension of the projection of the circulation chute (1) on the horizontal plane and the projection of the circulation chute feed pipe drop (4-1) on the horizontal plane is β; the outlet end of the external inclined tube (2) is provided with 1 external inclined tube feeding tube descending section (4-2), and the included angle between the extension line of the projection of the external inclined tube (2) on the horizontal plane and the projection of the external inclined tube feeding tube descending section (4-2) on the horizontal plane is beta; β = (180 ° - α)/2.
5. The device according to any one of claims 1-2, characterized in that the device comprises n circulation inclined pipes (1), n is more than or equal to 2; the included angle between the adjacent circulating inclined pipes (1) or the projections of the adjacent circulating inclined pipes (1) and the outer inclined pipe (2) on the horizontal plane is alpha ', alpha' =360 degrees/(n + 1).
6. The device of claim 5, wherein n = 2-10.
7. The apparatus according to claim 5, characterized in that the outlet end of each circulation chute (1) is provided with 2 circulation chute feed pipe drop sections (4-1), and the 2 circulation chute feed pipe drop sections (4-1) at the outlet end of each circulation chute (1) are symmetrical with respect to the extension line of the circulation chute (1); an included angle between the extension line of the projection of each circulation inclined pipe (1) on the horizontal plane and the projection of the descending section (4-1) of the circulation inclined pipe feeding pipe at the outlet end of the circulation inclined pipe on the horizontal plane is beta'; the outlet end of the external inclined tube (2) is provided with 2 external inclined tube feeding tube descending sections (4-2), and the 2 external inclined tube feeding tube descending sections (4-2) at the outlet end of the external inclined tube (2) are symmetrical according to the extension line of the external inclined tube (2); an included angle between an extension line of the projection of the external inclined tube (2) on the horizontal plane and the projection of a descending section (4-2) of the external inclined tube feeding tube at the outlet end of the external inclined tube on the horizontal plane is beta'; β '= (180 ° - α')/2.
8. The apparatus of claim 1, wherein the regenerator comprises a dense phase section and a lean phase section.
9. The apparatus according to claim 8, characterized in that the lean phase section of the regenerator is connected to the fast fluidized bed reactor (6) via a regeneration chute (3) and the dense phase section of the regenerator is connected to the dense bed (8) via a spent chute (9).
10. The device according to claim 1, characterized in that the regeneration chute horizontal section and the circulation chute horizontal section are arranged coaxially, the diameter of the regeneration chute (3) being smaller than the diameter of the circulation chute (1).
11. A method for producing olefins by catalytic conversion of methanol, which employs the apparatus according to any one of claims 1 to 10, comprising the steps of:
(a) methanol enters a fast fluidized bed reactor (6) to be fluidized and react with a catalyst, and the catalyst enters a secondary dense bed (8) along with gas phase material flow;
(b) the gas phase material flow is separated in a double dense bed (8) to obtain product gas and is discharged, and the catalyst is divided into three parts; the first strand is used as a circulating spent agent and returns to the fast fluidized bed reactor (6) through the circulating inclined pipe (1); the second part as an external spent agent returns to the fast fluidized bed reactor (6) through an external heat collector (7) and an external inclined tube (2); the third stream enters a regenerator (10) and returns to the fast fluidized bed reactor (6) as a regenerant through a regeneration inclined tube (3) after regeneration.
12. The process according to claim 11, characterized in that in step (b) the catalyst is divided into three streams, the first stream being returned as recycle spent agent to the fast fluidized bed reactor (6) through the recycle chute (1) via the recycle chute feed pipe drop (4-1); the second strand is taken as an external spent agent and returns to the fast fluidized bed reactor (6) through an external heat collector (7) and an external inclined tube (2) via an external inclined tube feeding pipe descending section (4-2); and the third strand enters a regenerator (10) through a to-be-regenerated inclined tube (9), is used as a regenerant after regeneration, enters the horizontal section of the circulating inclined tube (1) through a regeneration inclined tube (3) to be mixed with the circulating to-be-regenerated agent, is discharged through a descending section (4-1) of a feeding tube of the circulating inclined tube after being mixed with the circulating to-be-regenerated agent, and is then secondarily mixed with an externally-taken to-be-regenerated agent.
13. The process as claimed in claim 11 or 12, characterized in that the temperature in the fast-fluidized-bed reactor (6) is 400-500 ℃, 0.05-0.4MPaG of pressure and 2-20h of space velocity -1 。
14. The method as claimed in any one of claims 11 to 12, wherein the temperature of the circulating spent agent is 430-500 ℃; and/or the temperature of the external spent agent is 250-430 ℃; and/or the temperature of the regenerant is 500-700 ℃; and/or the feed flux of the circulating spent agent is 20-300kg/m 2 s; and/or the feeding flux of the external spent agent is 20-300kg/m 2 s; and/or the feed flux of the regenerant is from 20 to 300kg/m 2 s; and/or the recycling amount of the regenerant accounts for 1/30-1/10 of the total recycling amount.
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| CN103772105A (en) * | 2012-10-25 | 2014-05-07 | 中国石油化工股份有限公司 | Reaction device for improving yield of light olefins |
| CN207347423U (en) * | 2017-08-31 | 2018-05-11 | 中国石油化工股份有限公司 | Consersion unit |
| CN207581697U (en) * | 2017-08-31 | 2018-07-06 | 中国石油化工股份有限公司 | Reaction-regenerative device |
| CN109422617A (en) * | 2017-08-31 | 2019-03-05 | 中国石油化工股份有限公司 | Reaction-regenerative device and application thereof |
| CN109420468A (en) * | 2017-08-31 | 2019-03-05 | 中国石油化工股份有限公司 | Consersion unit and application thereof |
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|---|---|---|---|---|
| US7273960B2 (en) * | 2002-10-25 | 2007-09-25 | Exxonmobil Chemical Patents Inc | Fluid bed oxygenates to olefins reactor apparatus and process of controlling same |
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| CN103772105A (en) * | 2012-10-25 | 2014-05-07 | 中国石油化工股份有限公司 | Reaction device for improving yield of light olefins |
| CN203295445U (en) * | 2013-05-10 | 2013-11-20 | 中石化洛阳工程有限公司 | Regeneration catalyst distributor |
| CN207347423U (en) * | 2017-08-31 | 2018-05-11 | 中国石油化工股份有限公司 | Consersion unit |
| CN207581697U (en) * | 2017-08-31 | 2018-07-06 | 中国石油化工股份有限公司 | Reaction-regenerative device |
| CN109422617A (en) * | 2017-08-31 | 2019-03-05 | 中国石油化工股份有限公司 | Reaction-regenerative device and application thereof |
| CN109420468A (en) * | 2017-08-31 | 2019-03-05 | 中国石油化工股份有限公司 | Consersion unit and application thereof |
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