CN112619566A - Multistage jet loop reactor for preparing ethylene by oxidative coupling of methane - Google Patents
Multistage jet loop reactor for preparing ethylene by oxidative coupling of methane Download PDFInfo
- Publication number
- CN112619566A CN112619566A CN202110068239.2A CN202110068239A CN112619566A CN 112619566 A CN112619566 A CN 112619566A CN 202110068239 A CN202110068239 A CN 202110068239A CN 112619566 A CN112619566 A CN 112619566A
- Authority
- CN
- China
- Prior art keywords
- shell
- multistage
- methane
- gas distributor
- guide cylinder
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 title claims abstract description 67
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 title claims abstract description 32
- 239000005977 Ethylene Substances 0.000 title claims abstract description 32
- 238000005691 oxidative coupling reaction Methods 0.000 title claims abstract description 20
- 239000000463 material Substances 0.000 claims abstract description 40
- 239000003054 catalyst Substances 0.000 claims abstract description 13
- 239000007789 gas Substances 0.000 claims description 100
- 239000007921 spray Substances 0.000 claims description 22
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 20
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 14
- 239000001301 oxygen Substances 0.000 claims description 14
- 229910052760 oxygen Inorganic materials 0.000 claims description 14
- 239000000203 mixture Substances 0.000 claims description 13
- 229910052757 nitrogen Inorganic materials 0.000 claims description 10
- 238000006243 chemical reaction Methods 0.000 abstract description 19
- 238000009827 uniform distribution Methods 0.000 abstract description 3
- 230000009286 beneficial effect Effects 0.000 abstract description 2
- 239000007787 solid Substances 0.000 description 14
- 238000000926 separation method Methods 0.000 description 13
- 239000000047 product Substances 0.000 description 10
- 239000002994 raw material Substances 0.000 description 8
- 239000002245 particle Substances 0.000 description 7
- 238000000034 method Methods 0.000 description 6
- 238000004519 manufacturing process Methods 0.000 description 5
- 239000012528 membrane Substances 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- 238000005516 engineering process Methods 0.000 description 4
- 239000011949 solid catalyst Substances 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 238000009826 distribution Methods 0.000 description 3
- 239000006227 byproduct Substances 0.000 description 2
- 239000002826 coolant Substances 0.000 description 2
- 230000018109 developmental process Effects 0.000 description 2
- 229920006395 saturated elastomer Polymers 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 230000009471 action Effects 0.000 description 1
- 230000003321 amplification Effects 0.000 description 1
- 230000001276 controlling effect Effects 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000010790 dilution Methods 0.000 description 1
- 239000012895 dilution Substances 0.000 description 1
- 230000009977 dual effect Effects 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 239000005431 greenhouse gas Substances 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- 238000003199 nucleic acid amplification method Methods 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- 238000010791 quenching Methods 0.000 description 1
- 230000000171 quenching effect Effects 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 230000008844 regulatory mechanism Effects 0.000 description 1
- 238000010517 secondary reaction Methods 0.000 description 1
- 230000035945 sensitivity Effects 0.000 description 1
- 230000035939 shock Effects 0.000 description 1
Images
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
- B01J8/18—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles
- B01J8/20—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles with liquid as a fluidising medium
- B01J8/22—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles with liquid as a fluidising medium gas being introduced into the liquid
- B01J8/224—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles with liquid as a fluidising medium gas being introduced into the liquid the particles being subject to a circulatory movement
- B01J8/226—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles with liquid as a fluidising medium gas being introduced into the liquid the particles being subject to a circulatory movement internally, i.e. the particles rotate within the vessel
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C2/00—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms
- C07C2/76—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen
- C07C2/82—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen oxidative coupling
- C07C2/84—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen oxidative coupling catalytic
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- Combustion & Propulsion (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
- Devices And Processes Conducted In The Presence Of Fluids And Solid Particles (AREA)
Abstract
The invention relates to the technical field of methane conversion, in particular to a multistage jet circulation reactor for preparing ethylene by oxidative coupling of methane, which comprises a nozzle, a conical bottom, multistage guide cylinders, a gas distributor, a shell, a cyclone separator, a heat exchanger and a material returning device, wherein the nozzle is positioned at the bottom of the conical bottom, the conical bottom is positioned at the bottom end of the shell, the multistage guide cylinders are positioned at the middle lower part of the shell, the multistage guide cylinders are cylinders which are vertically arranged in equal diameter and have the quantity of more than or equal to 2, and the gas distributor is positioned at the middle lower part of the shell and has the quantity of 1 or more. The invention utilizes the nozzle, the conical bottom, the multi-stage guide cylinders and the gas distributor to form the forced internal circulation of materials, can promote the regular movement of the materials, reduce back mixing, strengthen mass transfer and heat transfer, is beneficial to the uniform distribution of the temperature in the reactor, and improves the utilization rate of the catalyst and the yield of the product.
Description
Technical Field
The invention relates to the technical field of methane conversion, in particular to a multistage jet loop reactor for preparing ethylene by oxidative coupling of methane.
Background
Ethylene is an important basic organic chemical product and raw material, and the production level is an important index for measuring the national chemical strength. At present, naphtha cracking is mainly used for ethylene production, and the problems of high cost and energy consumption, greenhouse gas emission and the like exist. With the development of international economy, ethylene production raw materials tend to be light and diversified. The technology for directly preparing ethylene by the one-step method of Oxidative Coupling of Methane (OCM) has the advantages of simple route, good economy and the like, is an ethylene production technology with wide development prospect, and has great significance for the optimization of energy structure in China.
The OCM reaction is a strong exothermic reaction at high temperature (750-950 ℃), and the ethylene yield has high sensitivity to temperature. How to remove the severe exotherm during the reaction is the key to engineering the technology. At present, OCM reactors mainly comprise fixed beds, fluidized beds, membrane reactors and the like.
The traditional fixed bed reactor has mature technology, measures such as multi-section cold shock, raw material quantity control and dilution gas addition are often used as an auxiliary measure in the implementation process to control the bed temperature, but the problem of difficult temperature control still exists in the actual production process aiming at the reaction characteristic of rapid strong heat release of OCM. Publication No. CN 106732201B discloses an OCM thin-layer fixed bed reactor, which comprises at least two sections of reaction section beds, wherein each section bed is composed of 1-2 layers of catalyst, the height is 20-40 mm, and each section of reaction section is connected through a quenching heat exchanger. Although the reactor overcomes the problem of axial temperature gradient, the radial direction still has the problems of uneven temperature distribution and the like, the temperature control among beds is more complicated, and the equipment and the operation cost are higher.
The fluidized bed can effectively strengthen the mass transfer and heat transfer process by utilizing the violent movement between gas and solid, and eliminate hot spots in the reactor. Publication No. CN 108530248A discloses an OCM fluidized bed device, which comprises a fluidizing zone and a settling zone, wherein the fluidizing zone comprises a heat exchanger and a gas distributor, and a plurality of cyclone separators are arranged in the settling zone. Although the reactor can effectively eliminate hot spots, gas in the reactor is seriously mixed back, which aggravates the secondary reaction process and influences the selectivity of ethylene.
Jaso (2011, 2011.03.23) proposed an auxiliary fluidized bed membrane reactor with oxygen feed rate controlled by the membrane to control reactor temperature and reaction degree. Although the membrane reactor can realize uniform distribution of temperature and high ethylene yield, the problems of membrane regeneration and pollution in industrialization are inevitable.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention provides a multistage jet loop reactor for preparing ethylene by oxidative coupling of methane, which aims to solve the problems of nonuniform temperature distribution, serious back mixing and low ethylene yield in the reactor.
The technical scheme adopted by the invention is as follows: a multi-stage jet circulation reactor for preparing ethylene by methane oxidative coupling comprises a nozzle (1), a conical bottom (2), a multi-stage guide cylinder, a gas distributor (5), a shell (3), a cyclone separator (9), a heat exchanger (11) and a material returning device, wherein the nozzle (1) is positioned at the bottom of the conical bottom (2), the conical bottom (2) is positioned at the bottom end of the shell (3), the multi-stage guide cylinder is positioned at the middle lower part of the shell (3) in number, the multi-stage guide cylinder is a cylinder which is vertically arranged in equal diameter and has the quantity more than or equal to 2, the gas distributor (5) is positioned at the middle lower part of the shell (3) and has the quantity of 1 or more, a gas outlet (7) at the top end of the shell (3) is connected with the upper part of the cyclone separator (9), a product gas outlet (8) is arranged at the top end of the cyclone separator (9), and the bottom of the, the middle of the dipleg (10) is provided with a heat exchanger (11), the dipleg (10) is communicated with a material returning device, and the material returning device comprises a material returning valve (12), a secondary air inlet (13), a discharge valve (14) and a material returning pipe (15).
One or more nozzles (1) are arranged, the jet air speed is 10-80 m/s, when one nozzle (1) is arranged, the nozzle (1) and the shell (3) are coaxial, when a plurality of nozzles (1) are arranged, the nozzles (1) are positioned on a circle on the axis of the central shell (3), and the maximum diameter of a circumscribed circle formed by each nozzle (1) is smaller than the diameter of the multistage guide cylinder.
The center lines of a plurality of cylinders contained in the multistage draft tube are overlapped, and the height of the cylinder positioned below is larger than or equal to that of the cylinder positioned above.
The ratio of the diameter of the multistage guide cylinder to the diameter of the shell (3) is 0.5-0.8; the ratio of the total height of the multi-stage guide cylinder to the height of the shell (3) is 0.4-0.7; the ratio of the distance from the bottom of the multistage draft tube to the bottom of the shell (3) to the diameter of the shell (3) is-0.3, and a negative value represents that the bottom of the lowest cylinder of the multistage draft tube is below the bottom of the shell (3).
The gas distributor is an annular gas distributor, and is one of a double annular gas distributor and a single annular gas distributor or a mixed combination of the double annular gas distributor and the single annular gas distributor.
The double-ring-shaped gas distributor is positioned at the interstage center of the multistage guide cylinder or the middle height of each cylinder of the multistage guide cylinder, the double-ring-shaped gas distributor consists of an inner ring-shaped distributor (17) and an outer ring-shaped distributor (20), the inner ring-shaped distributor (17) and the outer ring-shaped distributor (20) are connected through 4 guide pipes (19) which sequentially form 90 degrees, the inner ring-shaped distributor (17) is positioned in the multistage guide cylinder and vertically and upwardly uniformly distributed with upward spray holes (16), the outer ring-shaped distributor (20) is positioned between the multistage guide cylinder and the shell (3) and vertically and downwardly uniformly distributed with downward spray holes (21), the number of the upward spray holes (16) is more than or equal to 4 and less than or equal to that of the downward spray holes (21), and the number of the downward spray holes (21) is less than.
The single-ring-shaped gas distributor is positioned at the interstage center of the multi-stage guide cylinder and the middle height of each cylinder of the multi-stage guide cylinder, the diameter of the single-ring-shaped gas distributor positioned at the interstage center is smaller than that of the multi-stage guide cylinder, upward spray holes (16) are vertically and upwardly and uniformly distributed, the diameter of the single-ring-shaped gas distributor positioned at the middle height of each cylinder is between the diameters of the multi-stage guide cylinder and the shell (3), the downward spray holes (21) are vertically and downwardly and uniformly distributed, the number of the upward spray holes (16) is more than or equal to 4 and less than or equal to that of the downward spray holes (21), and the number of.
The secondary air inlet has two functional modes, namely an air inlet mode and a catalyst inlet mode.
The gas composition of the nozzle (1), the gas distributor (5) and the secondary air inlet (13) is a mixture of methane, oxygen and nitrogen.
The gas composition of the nozzle (1) is that the methane content is more than 90%, and the gas composition of the gas distributor and the secondary air inlet is that the oxygen content and the nitrogen content are more than 90%.
The cooling medium of the heat exchanger is saturated water or a mixture of water and steam, and high-quality steam can be produced as a byproduct.
The working principle of the multistage jet circulation reactor for preparing ethylene by oxidative coupling of methane comprises the following steps: according to the structure of the reactor, the reactor is divided into a conical bottom area, a circulating flow area, a gas-solid separation area, a cyclone separation area and a material returning area. The reaction raw material gas is sprayed into the conical bottom through the nozzle, the kinetic energy generated by the nozzle pushes catalyst particles to move upwards to enter the first-stage guide cylinder of the circulation zone, after the material leaves the first-stage guide cylinder, a part of the material continues to move upwards to enter the second-stage guide cylinder, a part of the material enters the first-stage guide cylinder and the shell annular space and moves downwards, a part of the material leaving the second-stage guide cylinder enters the gas-solid separation zone, and a part of the material returns to the second-stage guide cylinder and the shell annular space to participate in circulation. The concentration difference between the guide cylinder and the mixture of gas and particles in the annular space forms a circulating driving force, in addition, the circulation is strengthened by utilizing the different gas inlet directions of the inner ring and the outer ring of the gas distributor, and the oxygen concentration in the reactor is adjusted by adjusting the composition of the gas fed into the gas distributor. The orderly internal circulation of gas and solid can be forced through the action of injection and internal circulation flow, and the back mixing is reduced. The material entering the gas-solid separation zone is reduced in speed due to the widening of the flow channel, so that gas and solid catalyst are separated, the large-particle-size solid returns to the circulation zone, and the gas and the small-particle-size solid which is difficult to separate enter the cyclone separation zone for further separation. The product gas is discharged from the top of the cyclone separator, and the small-particle-size solid catalyst discharged from the bottom of the cyclone separator is cooled by a heat exchanger and then returns to the bottom of the reactor through a material returning area. The material returning area is provided with a secondary air inlet, and the product yield is assisted to be regulated and controlled by controlling the air inflow of the secondary air.
Compared with the prior art, the invention has the beneficial effects that:
1. the forced internal circulation of the materials is formed by the nozzle, the conical bottom, the multi-stage guide cylinders and the gas distributor, so that the regular movement of the materials can be promoted, the back mixing is reduced, the mass transfer and the heat transfer are enhanced, the uniform distribution of the temperature in the reactor is facilitated, and the utilization rate of the catalyst and the yield of the product are improved;
2. a three-stage gas regulation mechanism is formed by the nozzle, the gas distributor and the secondary air inlet, so that the oxygen concentration in the reactor is controlled, the deep reaction is effectively reduced, and the ethylene yield is improved;
3. the jet circulation reactor for preparing ethylene by oxidative coupling of methane has the advantages of simple structure, high operation flexibility and easy engineering amplification.
Drawings
FIG. 1 is a schematic diagram of the structure of an OCM multi-stage jet loop reactor;
FIG. 2 is a top view of a dual annular gas distributor;
FIG. 3 illustrates three possible annular gas distributor placements;
FIG. 4 is a top view of a single ring gas distributor (FIG. 3 (b));
wherein: 1-nozzle, 2-conical bottom, 3-shell, 4-first stage draft tube, 5-gas distributor, 6-second stage draft tube, 7-shell top gas outlet, 8-product gas outlet, 9-cyclone separator, 10-dipleg, 11-heat exchanger, 12-return valve, 13-secondary air inlet, 14-discharge valve, 15-return pipe, 16-upward spray hole, 17-inner ring distributor, 18-air inlet, 19-conduit, 20-outer ring distributor, and 21-downward spray hole.
Detailed Description
The invention is further described below with reference to the accompanying drawings.
Example 1
A multi-stage jet circulation reactor for preparing ethylene by oxidative coupling of methane is composed of conic bottom region, circulation region, gas-solid separation region, cyclone separation region and material returning region. The conical bottom zone comprises a nozzle 1 and a conical bottom 2; the circulation zone comprises a space at the middle lower part of the shell 3, a gas distributor 5, a first-stage guide cylinder 4 and a second-stage guide cylinder 6; the gas-solid separation zone comprises the upper space of the shell 3; the cyclonic separation zone comprises a cyclone 9; the material returning area comprises a dipleg 10, a heat exchanger 11, a material returning valve 12, a secondary air inlet 13, a discharge valve 14 and a material returning pipe 15.
As shown in fig. 1, the nozzle 1 is located at the bottom of the conical bottom 2, the conical bottom 2 is connected with the bottom of the shell 3, the first-stage guide cylinder 4 and the second-stage guide cylinder 6 are located at the middle lower part of the shell 3 and are vertically placed in sequence, the lower part of the shell 3 is provided with 1 or more gas distributors 5, the top of the shell 3 is provided with a gas outlet 7 and is connected with an inlet of a cyclone separator 9, the top of the cyclone separator 9 is provided with a product gas outlet 8, the bottom of the cyclone separator 9 is connected with a dipleg 10, the middle part of the dipleg 10 is provided with a heat exchanger 11 and is connected with a material returning valve 12 of a material returning device, the bottom of the dipleg 10 is provided with a discharge valve 14, a secondary air inlet 13 and a material returning pipe.
By adopting the placement of the annular gas distributor as shown in fig. 3 (a), in the specific implementation process, the reactor is heated to the reaction temperature before the start-up, the reaction raw material gas is sprayed into the conical bottom 2 through the nozzle 1, the catalyst is added to the target value through the secondary air inlet 13, and then the secondary air inlet 13 is switched to the air inlet mode. The kinetic energy generated by the nozzle 1 pushes catalyst particles to move upwards to enter the first-stage guide cylinder 4 of the circulation zone, after the materials leave the first-stage guide cylinder 4, a part of the materials continue to move upwards to enter the second-stage guide cylinder 6, a part of the materials enter annular gaps of the first-stage guide cylinder 4 and the shell 3 and move downwards, a part of the materials leaving the second-stage guide cylinder 6 enter a gas-solid separation zone, and a part of the materials return to the annular gaps of the second-stage guide cylinder 6 and the shell 3 to participate in circulation. The secondary raw material gas enters the double-ring-shaped gas distributor 5 through the gas inlet 18 and is redistributed through the inner ring-shaped distributor 17, the outer ring-shaped distributor 20 and the guide pipe 19 between the inner ring-shaped distributor and the outer ring-shaped distributor, one part of the redistributed secondary raw material gas is sprayed upwards from the upward spray holes 16 of the inner ring-shaped distributor 17 to enter the guide cylinder area, and the other part of the redistributed secondary raw material gas is sprayed downwards from the downward spray holes 21 of the outer ring-shaped distributor 20 to enter the annular space area. The concentration difference between the inside of the multistage draft tube and the mixture of gas and particles in the annular space forms a circulating driving force to promote the ordered internal circulation of the gas and the solids and reduce back mixing. The material entering the gas-solid separation zone is widened due to the flow channel and reduced in speed, so that gas and solid catalyst are separated, the large-particle-size solid returns to the circulation zone, the gas and the small-particle-size solid which is difficult to separate enter the cyclone separator 9 through the gas outlet 7 at the top end of the shell for further separation, the product gas is discharged from the product gas outlet 8 at the top end of the cyclone separator 9, and the small-particle-size solid catalyst is settled from the bottom of the cyclone separator 9, enters the dipleg 10, is cooled by the heat exchanger 11 and returns to the conical bottom 2 through the return pipe 15. The cooling medium in the heat exchanger 11 is saturated water or a mixture of water and steam to produce high-quality steam as a byproduct. In the operation process, the gas content of the nozzle 1, the gas distributor 5 and the secondary air inlet 13 is adjusted to regulate the product yield. When the catalyst needs to be replaced or supplemented, the secondary air inlet 13 can be switched into a catalyst inlet mode so as to realize the online non-stop operation.
The OCM jet loop reactor shown in figure 1 and figure 3 (a) is adopted, the average particle size of the catalyst is 100 μm, the reaction temperature is 800 ℃, the operation is carried out under normal pressure, the gas component passing through the nozzle is methane, the gas component passing through the gas distributor and the secondary air inlet is oxygen and nitrogen, the volume space velocity is 6000 h-1Methane: oxygen: nitrogen is present inThe methane conversion was 45% and the ethylene yield was 29% at a gas molar ratio of 3:1: 1.
Example 2
The same reactor configuration as in example 1 was used, except that: the annular gas distributor placement shown in fig. 3 (B) is adopted, and is particularly characterized in that the adopted annular gas distributor is a single annular gas distributor, wherein a single annular gas distributor with an upward opening (shown in fig. 4 (B-B)) is placed between stages of guide cylinders, and a single annular gas distributor with a downward opening (shown in fig. 4 (A-A)) is placed at the middle height of each guide cylinder. The average particle diameter of the catalyst is 100 μm, the reaction temperature is 800 ℃, the operation is carried out under normal pressure, the gas component passing through the nozzle is methane, the gas component passing through the gas distributor and the secondary air inlet is oxygen and nitrogen, and the volume space velocity is 6000 h-1Methane: oxygen: the methane conversion was 46% and the ethylene yield was 30% at a nitrogen molar ratio of 3:1: 1.
Example 3
The same reactor configuration as in example 1 was used, except that: the annular gas distributor placement mode shown in fig. 3 (c) is adopted, and specifically, the adopted double annular gas distribution mode is placed at the middle height of each guide shell. The average particle diameter of the catalyst is 150 μm, the reaction temperature is 800 ℃, the operation pressure is 5 bar, the gas components passing through the nozzle are methane and oxygen, the gas components passing through the gas distributor and the secondary air inlet are oxygen and nitrogen, and the volume space velocity is 8000 h-1Methane: oxygen: the methane conversion was 47% and the ethylene yield was 28% at a nitrogen molar ratio of 3:1: 1.
Claims (10)
1. A multi-stage jet circulation reactor for preparing ethylene by methane oxidative coupling is characterized in that: comprises a nozzle (1), a conical bottom (2), a multi-stage guide cylinder, a gas distributor (5), a shell (3), a cyclone separator (9), a heat exchanger (11) and a material returning device, wherein the nozzle (1) is positioned at the bottom of the conical bottom (2), the conical bottom (2) is positioned at the bottom of the shell (3), the multi-stage guide cylinder is positioned at the middle lower part of the shell (3) and is a cylinder with the same diameter and more than or equal to 2, the gas distributor (5) is positioned at the middle lower part of the shell (3) and is 1 or more, a shell top gas outlet (7) of the shell (3) is connected with the upper part of the cyclone separator (9), a product gas outlet (8) is arranged at the top of the cyclone separator (9), the bottom of the cyclone separator (9) is communicated with a material leg (10), the heat exchanger (11) is arranged in the middle of the material leg (10), and the material returning device is communicated with the material leg (10), the material returning device comprises a material returning valve (12), a secondary air inlet (13), a discharge valve (14) and a material returning pipe (15).
2. The multistage jet loop reactor for the oxidative coupling of methane to ethylene according to claim 1, wherein: one or more nozzles (1) are arranged, the jet air speed is 10-80 m/s, when one nozzle (1) is arranged, the nozzle (1) and the shell (3) are coaxial, when a plurality of nozzles (1) are arranged, the nozzles (1) are positioned on a circle on the axis of the central shell (3), and the maximum diameter of a circumscribed circle formed by each nozzle (1) is smaller than the diameter of the multistage guide cylinder.
3. The multistage jet loop reactor for the oxidative coupling of methane to ethylene according to claim 1, wherein: the center lines of a plurality of cylinders contained in the multistage draft tube are overlapped, and the height of the cylinder positioned below is larger than or equal to that of the cylinder positioned above.
4. The multistage jet loop reactor for the oxidative coupling of methane to ethylene according to claim 1, wherein: the ratio of the diameter of the multistage guide cylinder to the diameter of the shell (3) is 0.5-0.8; the ratio of the total height of the multi-stage guide cylinder to the height of the shell (3) is 0.4-0.7; the ratio of the distance from the bottom of the multistage draft tube to the bottom of the shell (3) to the diameter of the shell (3) is-0.3, and a negative value represents that the bottom of the lowest cylinder of the multistage draft tube is below the bottom of the shell (3).
5. The multistage jet loop reactor for the oxidative coupling of methane to ethylene according to claim 1, wherein: the gas distributor is an annular gas distributor, and is one of a double annular gas distributor and a single annular gas distributor or a mixed combination of the double annular gas distributor and the single annular gas distributor.
6. The multistage jet loop reactor for the oxidative coupling of methane to ethylene according to claim 5, wherein: the double-ring-shaped gas distributor is positioned at the interstage center of the multistage guide cylinder or the middle height of each cylinder of the multistage guide cylinder, the double-ring-shaped gas distributor consists of an inner ring-shaped distributor (17) and an outer ring-shaped distributor (20), the inner ring-shaped distributor (17) and the outer ring-shaped distributor (20) are connected through 4 guide pipes (19) which sequentially form 90 degrees, the inner ring-shaped distributor (17) is positioned in the multistage guide cylinder and vertically and upwardly uniformly distributed with upward spray holes (16), the outer ring-shaped distributor (20) is positioned between the multistage guide cylinder and the shell (3) and vertically and downwardly uniformly distributed with downward spray holes (21), the number of the upward spray holes (16) is more than or equal to 4 and less than or equal to that of the downward spray holes (21), and the number of the downward spray holes (21) is less than.
7. The multistage jet loop reactor for the oxidative coupling of methane to ethylene according to claim 5, wherein: the single-ring-shaped gas distributor is positioned at the interstage center of the multi-stage guide cylinder and the middle height of each cylinder of the multi-stage guide cylinder, the diameter of the single-ring-shaped gas distributor positioned at the interstage center is smaller than that of the multi-stage guide cylinder, upward spray holes (16) are vertically and upwardly and uniformly distributed, the diameter of the single-ring-shaped gas distributor positioned at the middle height of each cylinder is between the diameters of the multi-stage guide cylinder and the shell (3), the downward spray holes (21) are vertically and downwardly and uniformly distributed, the number of the upward spray holes (16) is more than or equal to 4 and less than or equal to that of the downward spray holes (21), and the number of.
8. The multistage jet loop reactor for the oxidative coupling of methane to ethylene according to claim 1, wherein: the secondary air inlet has two functional modes, namely an air inlet mode and a catalyst inlet mode.
9. The multistage jet loop reactor for the oxidative coupling of methane to ethylene according to claim 1, wherein: the gas composition of the nozzle (1), the gas distributor (5) and the secondary air inlet (13) is a mixture of methane, oxygen and nitrogen.
10. The multistage jet loop reactor for the oxidative coupling of methane to ethylene according to claim 1, wherein: the gas composition of the nozzle (1) is that the methane content is more than 90%, and the gas composition of the gas distributor and the secondary air inlet is that the oxygen content and the nitrogen content are more than 90%.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202110068239.2A CN112619566B (en) | 2021-01-19 | 2021-01-19 | Multistage jet loop reactor for preparing ethylene by oxidative coupling of methane |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202110068239.2A CN112619566B (en) | 2021-01-19 | 2021-01-19 | Multistage jet loop reactor for preparing ethylene by oxidative coupling of methane |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN112619566A true CN112619566A (en) | 2021-04-09 |
| CN112619566B CN112619566B (en) | 2022-04-12 |
Family
ID=75294517
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN202110068239.2A Active CN112619566B (en) | 2021-01-19 | 2021-01-19 | Multistage jet loop reactor for preparing ethylene by oxidative coupling of methane |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN112619566B (en) |
Citations (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1143064A (en) * | 1996-07-12 | 1997-02-19 | 天津大学 | Method for sulfonating liquid state organics by gas phase sulfur trioxide and its equipment |
| CN1435275A (en) * | 2002-02-01 | 2003-08-13 | 中国石油天然气股份有限公司 | Multi-stage circular flow reactor |
| CN101274245A (en) * | 2007-03-28 | 2008-10-01 | 中国石油大学(北京) | Annular space air-lift gas-solid loop flow reactor |
| WO2015081122A2 (en) * | 2013-11-27 | 2015-06-04 | Siluria Technologies, Inc. | Reactors and systems for oxidative coupling of methane |
| CN105505749A (en) * | 2016-03-04 | 2016-04-20 | 江南大学 | Air-liquid dual injection type airlift loop reactor |
| CN105694959A (en) * | 2016-02-03 | 2016-06-22 | 浙江大学 | Jet-type internal circulation flow reactor for heavy oil hydrocracking |
| CN106582459A (en) * | 2015-10-15 | 2017-04-26 | 中国石油化工股份有限公司 | Fluidized bed reactor, lower-carbon olefin preparation apparatus, and lower-carbon olefin preparation method |
| CN107930540A (en) * | 2017-11-07 | 2018-04-20 | 四川金象赛瑞化工股份有限公司 | A kind of controlling temp type multilayer FCC reactor |
| WO2018072139A1 (en) * | 2016-10-19 | 2018-04-26 | 中国科学院大连化学物理研究所 | Turbulent fluidized-bed reactor, device, and method using oxygen-containing compound for manufacturing propene and c4 hydrocarbon |
| CN109012513A (en) * | 2018-08-16 | 2018-12-18 | 中国石油大学(北京) | A kind of methanol to olefins reaction device |
| CN110227394A (en) * | 2019-04-24 | 2019-09-13 | 中国科学院山西煤炭化学研究所 | A kind of fluidized-bed reactor for Catalyst for Oxidative Coupling of Methane |
| CN211800720U (en) * | 2019-12-24 | 2020-10-30 | 洛阳融惠化工科技有限公司 | Gas lift type circulating fluidized bed loop reactor for preparing olefin from methanol |
| WO2020220586A1 (en) * | 2019-04-29 | 2020-11-05 | 中国矿业大学 | Mixture separation system and method employing fluid enhancement |
-
2021
- 2021-01-19 CN CN202110068239.2A patent/CN112619566B/en active Active
Patent Citations (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1143064A (en) * | 1996-07-12 | 1997-02-19 | 天津大学 | Method for sulfonating liquid state organics by gas phase sulfur trioxide and its equipment |
| CN1435275A (en) * | 2002-02-01 | 2003-08-13 | 中国石油天然气股份有限公司 | Multi-stage circular flow reactor |
| CN101274245A (en) * | 2007-03-28 | 2008-10-01 | 中国石油大学(北京) | Annular space air-lift gas-solid loop flow reactor |
| WO2015081122A2 (en) * | 2013-11-27 | 2015-06-04 | Siluria Technologies, Inc. | Reactors and systems for oxidative coupling of methane |
| CN106582459A (en) * | 2015-10-15 | 2017-04-26 | 中国石油化工股份有限公司 | Fluidized bed reactor, lower-carbon olefin preparation apparatus, and lower-carbon olefin preparation method |
| CN105694959A (en) * | 2016-02-03 | 2016-06-22 | 浙江大学 | Jet-type internal circulation flow reactor for heavy oil hydrocracking |
| CN105505749A (en) * | 2016-03-04 | 2016-04-20 | 江南大学 | Air-liquid dual injection type airlift loop reactor |
| WO2018072139A1 (en) * | 2016-10-19 | 2018-04-26 | 中国科学院大连化学物理研究所 | Turbulent fluidized-bed reactor, device, and method using oxygen-containing compound for manufacturing propene and c4 hydrocarbon |
| CN107930540A (en) * | 2017-11-07 | 2018-04-20 | 四川金象赛瑞化工股份有限公司 | A kind of controlling temp type multilayer FCC reactor |
| CN109012513A (en) * | 2018-08-16 | 2018-12-18 | 中国石油大学(北京) | A kind of methanol to olefins reaction device |
| CN110227394A (en) * | 2019-04-24 | 2019-09-13 | 中国科学院山西煤炭化学研究所 | A kind of fluidized-bed reactor for Catalyst for Oxidative Coupling of Methane |
| WO2020220586A1 (en) * | 2019-04-29 | 2020-11-05 | 中国矿业大学 | Mixture separation system and method employing fluid enhancement |
| CN211800720U (en) * | 2019-12-24 | 2020-10-30 | 洛阳融惠化工科技有限公司 | Gas lift type circulating fluidized bed loop reactor for preparing olefin from methanol |
Also Published As
| Publication number | Publication date |
|---|---|
| CN112619566B (en) | 2022-04-12 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN101274245B (en) | Annular space air-lift gas-solid loop flow reactor | |
| CN105505441A (en) | Catalytic cracking reaction regeneration method and device | |
| CN103540345B (en) | Catalytic cracking method | |
| CN109012513B (en) | Methanol-to-olefin reactor | |
| CN104437274B (en) | Fluidized bed reactor used for light olefin cracking and Methanol To Olefin (MTO) | |
| CN112973579B (en) | Gas-solid short contact time reaction device and application thereof | |
| CN111807916B (en) | Device for producing low-carbon olefin by efficient oxygen-containing compound | |
| CN110078580B (en) | Fluidized bed reaction device and method for preparing ethylene through oxidative coupling of methane | |
| CN109433116B (en) | Shell-and-tube axial tube reactor for strong exothermic chemical reaction process | |
| WO2015149646A1 (en) | Fluidized bed apparatus and method for preparing polymethoxy dimethylether from methylal and paraformaldehyde | |
| CN103540346B (en) | A kind of Desending catalytic cracking device | |
| CN103341341A (en) | Fluidized bed reactor for preparing butadiene | |
| CN203355710U (en) | Rapid fluidized bed reactor for producing butadiene by butylene oxydehydrogenation | |
| CN1058046C (en) | Catalyst cracking method for producing in high-yield olefin and lift-leg reaction system thereof | |
| CN112619566B (en) | Multistage jet loop reactor for preparing ethylene by oxidative coupling of methane | |
| CN111875465B (en) | Method for producing low-carbon olefin by oxygen-containing compound | |
| CN112808181B (en) | Jet loop reactor for preparing ethylene by oxidative coupling of methane | |
| CN103788993B (en) | A kind of catalytic cracking unit | |
| CN111054277A (en) | Reactor and method for producing low-carbon olefin | |
| CN111875464B (en) | Method for producing low-carbon olefin by high-efficiency oxygen-containing compound | |
| CN112973584B (en) | Fluidized bed reaction device and application thereof | |
| CN1140607C (en) | apparatus for producing low carbon olefines by high-tmep. catalyzing contact cracking from heavy petroleum hydrocarbon | |
| CN112708447B (en) | Riser reactor capable of reducing back mixing of side wall area | |
| CN202983653U (en) | Fluidized bed reactor for preparing butadiene by oxidizing and dehydrogenizing butene | |
| CN114425248B (en) | Catalytic converter mixer, device for producing low-carbon olefin and method and application for producing low-carbon olefin |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| TA01 | Transfer of patent application right | ||
| TA01 | Transfer of patent application right |
Effective date of registration: 20220308 Address after: 046200 Wangqiao Industrial Park, Xiangyuan County, Changzhi City, Shanxi Province Applicant after: Shanxi Lu'an Chemical Co.,Ltd. Applicant after: Shanxi Institute of coal chemistry, Chinese Academy of Sciences Address before: 030001 No. 27 Taoyuan South Road, Shanxi, Taiyuan Applicant before: INSTITUTE OF COAL CHEMISTRY, CHINESE ACADEMY OF SCIENCES |
|
| GR01 | Patent grant | ||
| GR01 | Patent grant |