CN117339487A - Reaction device and method for efficiently converting synthesis gas - Google Patents
Reaction device and method for efficiently converting synthesis gas Download PDFInfo
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- CN117339487A CN117339487A CN202311253203.7A CN202311253203A CN117339487A CN 117339487 A CN117339487 A CN 117339487A CN 202311253203 A CN202311253203 A CN 202311253203A CN 117339487 A CN117339487 A CN 117339487A
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- 238000006243 chemical reaction Methods 0.000 title claims abstract description 107
- 230000015572 biosynthetic process Effects 0.000 title claims abstract description 79
- 238000003786 synthesis reaction Methods 0.000 title claims abstract description 79
- 238000000034 method Methods 0.000 title claims abstract description 37
- 239000007789 gas Substances 0.000 claims abstract description 203
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 43
- 150000001336 alkenes Chemical class 0.000 claims abstract description 40
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 claims abstract description 38
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 33
- 239000001257 hydrogen Substances 0.000 claims abstract description 32
- 230000003197 catalytic effect Effects 0.000 claims abstract description 25
- 238000010438 heat treatment Methods 0.000 claims abstract description 24
- 229910001868 water Inorganic materials 0.000 claims abstract description 24
- 239000003054 catalyst Substances 0.000 claims description 85
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical group [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 52
- 239000002245 particle Substances 0.000 claims description 31
- 229910052742 iron Inorganic materials 0.000 claims description 26
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 23
- 239000002184 metal Substances 0.000 claims description 20
- 229910052751 metal Inorganic materials 0.000 claims description 20
- 229930195733 hydrocarbon Natural products 0.000 claims description 18
- 150000002430 hydrocarbons Chemical class 0.000 claims description 18
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 15
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 15
- 229910052802 copper Inorganic materials 0.000 claims description 15
- 239000010949 copper Substances 0.000 claims description 15
- 238000004064 recycling Methods 0.000 claims description 14
- 150000002431 hydrogen Chemical class 0.000 claims description 8
- 229910017052 cobalt Inorganic materials 0.000 claims description 7
- 239000010941 cobalt Substances 0.000 claims description 7
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 7
- 239000011148 porous material Substances 0.000 claims description 5
- 238000007599 discharging Methods 0.000 claims description 4
- 238000011049 filling Methods 0.000 claims description 2
- 238000000926 separation method Methods 0.000 abstract description 19
- 230000008901 benefit Effects 0.000 abstract description 8
- 125000004435 hydrogen atom Chemical class [H]* 0.000 abstract 1
- 239000000047 product Substances 0.000 description 47
- 239000004215 Carbon black (E152) Substances 0.000 description 12
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 12
- 229910052799 carbon Inorganic materials 0.000 description 10
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 8
- 239000000463 material Substances 0.000 description 6
- 239000007795 chemical reaction product Substances 0.000 description 5
- 238000010586 diagram Methods 0.000 description 5
- 239000012467 final product Substances 0.000 description 5
- 239000000203 mixture Substances 0.000 description 4
- 239000002994 raw material Substances 0.000 description 4
- 239000003245 coal Substances 0.000 description 3
- 238000005265 energy consumption Methods 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 238000002360 preparation method Methods 0.000 description 3
- KAKZBPTYRLMSJV-UHFFFAOYSA-N Butadiene Chemical compound C=CC=C KAKZBPTYRLMSJV-UHFFFAOYSA-N 0.000 description 2
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 2
- 239000005977 Ethylene Substances 0.000 description 2
- 239000003153 chemical reaction reagent Substances 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 150000002894 organic compounds Chemical class 0.000 description 2
- 239000003208 petroleum Substances 0.000 description 2
- -1 polyethylene Polymers 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 1
- 239000004698 Polyethylene Substances 0.000 description 1
- 230000000903 blocking effect Effects 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
- 230000005494 condensation Effects 0.000 description 1
- 238000007334 copolymerization reaction Methods 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 238000006356 dehydrogenation reaction Methods 0.000 description 1
- 230000001419 dependent effect Effects 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 239000012847 fine chemical Substances 0.000 description 1
- 238000002309 gasification Methods 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 239000012567 medical material Substances 0.000 description 1
- 239000004033 plastic Substances 0.000 description 1
- 229920003023 plastic Polymers 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 1
- 230000003252 repetitive effect Effects 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- 239000004711 α-olefin Substances 0.000 description 1
Classifications
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- 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
- B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
-
- 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
- B01J8/001—Controlling catalytic processes
-
- 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
- B01J8/0015—Feeding of the particles in the reactor; Evacuation of the particles out of the reactor
-
- 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
- B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
- B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
-
- 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
- B01J8/24—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles according to "fluidised-bed" technique
-
- 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
- B01J8/24—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles according to "fluidised-bed" technique
- B01J8/26—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with fluidised particles according to "fluidised-bed" technique with two or more fluidised beds, e.g. reactor and regeneration installations
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/06—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents
- C01B3/12—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents by reaction of water vapour with carbon monoxide
-
- 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
- B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
- B01J2208/00008—Controlling the process
-
- 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
- B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
- B01J2208/00008—Controlling the process
- B01J2208/00017—Controlling the temperature
- B01J2208/00026—Controlling or regulating the heat exchange system
- B01J2208/00035—Controlling or regulating the heat exchange system involving measured parameters
- B01J2208/00044—Temperature measurement
-
- 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
- B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
- B01J2208/00008—Controlling the process
- B01J2208/00654—Controlling the process by measures relating to the particulate material
- B01J2208/00672—Particle size selection
Abstract
The invention provides a reaction device and a method for efficiently converting synthesis gas, wherein the device comprises a primary reactor and a secondary reactor; the primary reactor and the secondary reactor are separated by a porous plate; the primary reactor is used for carrying out catalytic conversion on the synthesis gas to obtain mixed gas containing olefin; the secondary reactor is used for carrying out catalytic conversion on unreacted CO in the primary reactor and water vapor generated by the reaction to generate hydrogen, and finally obtaining CO-free product gas; the primary reactor is provided with a heating device, and the secondary reactor is provided with a heat exchange device to realize independent temperature control. The reaction device provided by the invention enables the synthesis gas to be converted into olefin to the greatest extent, meanwhile, the product does not contain CO, and the water content in the product is greatly reduced, so that the separation procedure of olefin in the later stage is simplified. Has the advantages of short flow and low cost.
Description
Technical Field
The invention relates to the technical field of clean coal chemical industry and clean natural gasification industry, in particular to a reaction device and a method for efficiently converting synthesis gas.
Background
Olefin is one of the most important chemical raw materials, and provides a foundation for synthesizing various plastics, fibers, medical materials and the like. For example, the current ethylene and propylene yields in China are over 5000 ten thousand tons/year, and the butadiene yields are over 600 ten thousand tons/year; the high carbon number alpha olefin is used for the copolymerization of polyethylene and the production of various fine chemicals to construct a huge product network of chemistry and materials. Currently, olefins are mainly obtained by cracking petroleum feedstocks, other evolving routes include the production of olefins from coal via methanol, and the production of ethylene by ethane dehydrogenation. The bottleneck in petroleum routes is resource dependent. The method for preparing olefin from coal by methanol has the characteristics of long route, large equipment investment and enlarged carbon emission.
In comparison, the method directly prepares the olefin from the synthesis gas without methanol, and has the advantages of short route and low investment. However, the CO conversion is incomplete, the product separation step is complicated, and the material consumption and the energy consumption of recycling the hydrogen in the product are high.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides a reaction device and a method for efficiently converting synthesis gas, which enable the synthesis gas to be converted into olefin to the greatest extent, simultaneously enable the product to contain no CO or little CO, reduce the water content in the product, and simplify the separation process of olefin in the later stage. Has the advantages of short flow and low cost.
The specific invention comprises the following steps:
in a first aspect, the present invention provides a reaction apparatus for efficient conversion of synthesis gas, the apparatus comprising a primary reactor and a secondary reactor; the primary reactor and the secondary reactor are separated by a porous plate;
the primary reactor is used for carrying out catalytic conversion on the synthesis gas to obtain mixed gas containing olefin;
the secondary reactor is used for carrying out catalytic conversion on unreacted CO in the primary reactor and water vapor generated by the reaction to generate hydrogen, and finally obtaining CO-free product gas;
the primary reactor is provided with a heating device, and the secondary reactor is provided with a heat exchange device to realize independent temperature control.
Alternatively, the primary reactor is configured as a fixed bed or fluidized bed and the secondary reactor is configured as a fixed bed or fluidized bed.
Optionally, the primary reactor and the secondary reactor are both configured as fixed beds.
Optionally, a feed gas inlet is arranged at the bottom of the primary reactor; the top of the secondary reactor is provided with a product gas outlet;
the secondary reactor is provided with two catalyst filling ports which are respectively close to the porous plate and the product gas outlet.
In a second aspect, the present invention provides a method for efficiently converting synthesis gas, the method being suitable for use in a reaction apparatus according to the first aspect, the method comprising the steps of:
s1, introducing synthesis gas into a first-stage reactor through a feed gas inlet, and reacting the synthesis gas under the action of a metal-based catalyst to obtain mixed gas containing olefin; the mixed gas comprises water vapor, CO and CO 2 And C1-C7 hydrocarbons;
s2, enabling the mixed gas to enter a secondary reactor through pores of a porous plate, and carrying out catalytic conversion on CO and steam in the mixed gas under the action of a water gas catalyst to generate hydrogen so as to obtain CO-free product gas;
s3, discharging the product gas out of the secondary reactor through a product gas outlet, and separating to obtain hydrogen and target product olefin; the hydrogen is further used for configuring the synthesis gas for recycling.
Optionally, in step S1, the temperature in the primary reactor is controlled by a heating device, and the temperature is 240-280 ℃;
the metal-based catalyst is an iron-based catalyst or a cobalt-based catalyst;
when the primary reactor is a fixed bed, the particle size of the metal-based catalyst is 0.3-6mm;
when the primary reactor is a fluidized bed, the particle size of the metal-based catalyst is 0.03-0.3mm.
Optionally, in step S2, the temperature in the secondary reactor is controlled by a heat exchange device, and the temperature is 180-220 ℃;
the water gas catalyst is an iron-based catalyst or a copper-based catalyst;
when the secondary reactor is a fixed bed, the particle size of the metal-based catalyst is 0.3-6mm;
when the secondary reactor is a fluidized bed, the particle size of the metal-based catalyst is 0.03-0.3mm.
Optionally, in step S1, the space velocity of the synthesis gas ranges from 1000 to 10000ml/gcat/h.
Optionally, in step S2, the space velocity of the mixed product 1 in the secondary reactor is 1000-20000ml/gcat/h.
Optionally, in the synthesis gas, H 2 The volume ratio of the catalyst to CO is 1.25:1-2.5:1.
Compared with the prior art, the invention has the following advantages:
the invention provides a reaction device for efficiently converting synthesis gas, which comprises a primary reactor and a secondary reactor; the primary reactor and the secondary reactor are separated by a porous plate; the primary reactor is used for carrying out catalytic conversion on the synthesis gas to obtain mixed gas containing olefin; the secondary reactor is used for carrying out catalytic conversion on the unreacted CO in the primary reactor and the water vapor generated by the reaction to generate hydrogen, and finally obtaining the product gas without the CO and the water vapor; the primary reactor is provided with a heating device, and the secondary reactor is provided with a heat exchange device to realize independent temperature control. The reaction device provided by the invention enables the synthesis gas to be converted into olefin to the greatest extent, meanwhile, the product does not contain CO, and the water content in the product is greatly reduced, so that the separation procedure of olefin in the later stage is simplified. Has the advantages of short flow and low cost.
The invention also provides a method for synthesizingMethod for high-efficiency conversion of gas, which makes synthesis gas react under the action of metal-based catalyst by means of primary reactor to obtain catalyst composed of water vapor, CO and CO 2 And the mixed gas is further subjected to catalytic treatment in a secondary reactor, so that CO in the mixed gas and water vapor are subjected to catalytic conversion to generate hydrogen, and CO in the product is removed. Since the product gas outlet of the secondary reactor contains little CO and water, the subsequent separation device is reduced by 33%. The investment cost is reduced by 25 percent, and the running cost is reduced by 20 percent. And because the mixed gas carries a large amount of heat energy, when entering the secondary reactor for further reaction, the heat energy is not required to be additionally provided for further conversion of water vapor and CO in the mixed gas, and the heat exchange device is used for effectively controlling the secondary reactor to supply heat for the secondary reactor by utilizing the reaction heat in the primary reactor, so that the energy saving and emission reduction targets are realized. The separated hydrogen can be directly used for configuration of synthesis gas, so that recycling of the hydrogen is realized. Compared with the method without conversion of a secondary reactor, the method directly utilizes the hydrogen in the mixed product 1, avoids the material consumption and the energy consumption which are spent in the preparation of the hydrogen-carbon ratio, and can save the cost by 20 percent.
Drawings
In order to more clearly illustrate the embodiments of the invention or the technical solutions in the prior art, the drawings that are required in the embodiments or the description of the prior art will be briefly described, it being obvious that the drawings in the following description are only some embodiments of the invention, and that other drawings may be obtained according to these drawings without inventive effort for a person skilled in the art.
FIG. 1 shows a schematic diagram of a reaction apparatus for efficient conversion of synthesis gas provided by an embodiment of the present invention;
FIG. 2 shows a schematic diagram of another reaction apparatus for efficient conversion of synthesis gas according to an embodiment of the present invention
FIG. 3 shows a schematic diagram of another reaction apparatus for efficient conversion of synthesis gas provided by an embodiment of the present invention;
FIG. 4 shows a flow chart of a method for efficiently converting synthesis gas provided by an embodiment of the invention.
Wherein reference numerals are intended to: 1-a reaction apparatus body; 2-a first stage reactor; a 3-secondary reactor; 4-a porous plate; 5-a heating device; 6-a heat exchange device; 7, a raw material gas inlet; 8-product gas outlet.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings in the embodiments of the present invention. It will be apparent that the described embodiments are only some, but not all, embodiments of the invention. The following description of at least one exemplary embodiment is merely exemplary in nature and is in no way intended to limit the invention, its application, or uses. Any product that is the same as or similar to the present invention, which anyone in the light of the present invention or combines the present invention with other prior art features, falls within the scope of the present invention based on the embodiments of the present invention. And all other embodiments that may be made by those of ordinary skill in the art without undue burden and without departing from the scope of the invention.
Specific experimental steps or conditions are not noted in the examples and may be performed in accordance with the operation or conditions of conventional experimental steps described in the prior art in the field. The reagents used, as well as other instruments, are conventional reagent products available commercially, without the manufacturer's knowledge. Furthermore, the drawings are merely schematic illustrations of embodiments of the invention and are not necessarily drawn to scale. The same reference numerals in the drawings denote the same or similar parts, and thus a repetitive description thereof will be omitted. Some of the block diagrams shown in the figures are functional entities and do not necessarily correspond to physically or logically separate entities.
Techniques, methods and apparatus known to those of ordinary skill in the relevant art may not be discussed in detail, but are intended to be part of the present description where appropriate.
In the description of the present invention, it should be understood that the terms "first," "second," and the like are used for defining the components, and are merely for convenience in distinguishing the corresponding components, and the terms are not meant to have any special meaning unless otherwise indicated, so that the scope of the present invention is not to be construed as being limited.
In addition, the technical features of the different embodiments of the present invention described below may be combined with each other as long as they do not collide with each other.
Before describing in detail a reaction apparatus and a method for efficiently converting synthesis gas according to the present invention, the following description is necessary for the related art:
in the prior art, the reaction product obtained by directly preparing olefin from synthesis gas without methanol comprises C1-C7 organic compounds, water, hydrogen, CO and CO 2 The multiple components make the separation process complicated and cumbersome. For example, in the separation of C4-C7 by condensation, water may condense with liquid hydrocarbons such as C4-C7, which makes separation difficult. As another example, the molecular weight of the residual CO in the reaction product is close to that of the C2-C3 hydrocarbons, which results in a complex separation sequence of the C2-C3 hydrocarbons. In addition, the mixture ratio of the synthesis gas, which is the raw material gas for most reactions, is CO excess and H 2 Insufficient content, thus CO and H in the reaction product 2 Recycling is also caused by H in the reaction product 2 Insufficient content results in failure to achieve the intended recycling benefit.
Based on the problems, the invention provides a reaction device and a method for efficiently converting synthesis gas into olefin, so that the synthesis gas is converted into olefin to the greatest extent, meanwhile, the product contains no CO or little CO, the content of water in the product is reduced, the separation process of the olefin at the later stage is effectively simplified, and the utilization value of hydrogen in the product is improved. The preparation method has the advantages of short flow and low cost. The specific implementation content is as follows:
in a first aspect, the present invention provides a reaction device for efficiently converting synthesis gas, fig. 1 shows a schematic diagram of a reaction device for efficiently converting synthesis gas provided in an embodiment of the present invention, and as shown in fig. 1, a reaction device body 1 specifically includes a primary reactor 2 and a secondary reactor 3; the primary reactor 2 and the secondary reactor 3 are separated by a porous plate 4; as can be seen from fig. 1, the reactor body 1 can also be regarded as a reactor body 1 divided into two sections by a porous plate 4 to form a primary reactor 2 and a secondary reactor 3, wherein gas in the primary reactor 2 can enter the secondary reactor 3 through the pores on the porous plate 4, and a catalyst filled in the primary reactor 2 cannot enter the secondary reactor 3 due to the blocking of the porous plate 4, so that the primary reactor 2 and the secondary reactor 3 can maintain relatively independent reaction spaces.
The synthesis gas entering the primary reactor 2 is subjected to catalytic conversion under the action of high temperature and a catalyst to generate C1-C7 organic compounds containing olefin, water vapor, hydrogen, CO and CO 2 Hereinafter, the mixture of the above gases is collectively referred to as a mixed gas. The mixed gas enters the secondary reactor 3 through the pores on the porous plate 4, and in the secondary reactor 3, CO and water vapor in the mixed gas are further subjected to catalytic conversion under the conditions of a catalyst and a temperature lower than that in the primary reactor 2, so that hydrogen is generated, CO in an end product is removed, and finally, the product gas without CO and water vapor is obtained.
With continued reference to FIG. 1, the primary reactor 2 is provided with a heating device 5 to maintain the temperature in the primary reactor 2 at 250-350 ℃ to support catalytic conversion of the synthesis gas; because the temperature required by the water gas shift reaction (reaction of CO and water vapor) carried out in the secondary reactor 3 is lower than the catalytic conversion temperature of the synthesis gas (the temperature difference is about 100 ℃), and the mixed gas flowing from the primary reactor 2 to the secondary reactor 3 carries heat, no additional heat energy is required to be provided for the water gas shift reaction carried out in the secondary reactor 3, namely no additional heating device is required, only the heat exchange device 6 containing a condensing part is arranged, the temperature in the secondary reactor 3 is controlled to be maintained at 180-220 ℃, and the arrangement of the heating device 5 and the heat exchange device 6 enables the two reactors to realize independent temperature control and simultaneously reduces the heat energy consumed by the efficient conversion of the synthesis gas.
In some embodiments, the primary reactor 2 may be any one of a fixed bed and a fluidized bed, and the secondary reactor 3 may also be any one of a fixed bed and a fluidized bed. Specifically, in the reactor body 1 shown in fig. 1, the primary reactor 2 and the secondary reactor 3 are both configured as fixed beds; in the reactor body 1 shown in fig. 2, the primary reactor 2 and the secondary reactor 3 are both configured as fluidized beds, and in the reactor body 1 shown in fig. 3, the primary reactor 2 is configured as a fluidized bed, and the secondary reactor 3 is configured as a fixed bed. When the primary reactor 2 is configured as a fluidized bed, the provision of the particle trapping device may be omitted, resulting in an increase in the space utilization of the primary reactor 2.
In some embodiments, the bottom of the primary reactor 2 is provided with a feed gas inlet 7 to facilitate entry of feed gas into the reactor; the top of the secondary reactor 3 is provided with a product gas outlet 8 for discharging product gas out of the reactor.
Further, the catalyst charge port of the primary reactor 2 is provided close to the heating device 5 (not shown in the figure); the secondary reactor is provided with two catalyst loading ports, which are arranged close to the porous plate 4 and the product gas outlet 8, respectively. So that the water gas shift reaction is fully carried out and the CO in the product gas discharged from the product gas outlet 8 is ensured to be removed completely.
The reaction device provided by the invention enables the synthesis gas to be converted into olefin to the greatest extent, meanwhile, the product does not contain CO, and the water content in the product is greatly reduced, so that the separation procedure of olefin in the later stage is simplified. Has the advantages of short flow and low cost.
In a second aspect, the present invention provides a method for efficiently converting synthesis gas, where the method is applicable to the reaction apparatus of the first aspect, and fig. 4 shows a flowchart of a method for efficiently converting synthesis gas provided by an embodiment of the present invention, and as shown in fig. 4, the method includes the following steps:
s1, introducing synthesis gas into a first-stage reactor 2 through a feed gas inlet 7, and reacting the synthesis gas under the action of a metal-based catalyst to obtain a mixed gas containing olefin, wherein the mixed gas comprises water vapor, CO and CO 2 And C1-C7 hydrocarbons;
specifically, the airspeed of the synthesis gas fed into the primary reactor 2 is 1000-10000ml/gcat/h; the temperature in the primary reactor 2 is controlled by a heating device 5, and the temperature is 240-280 ℃; the metal-based catalyst is an iron-based catalyst or a cobalt-based catalyst; and, when the primary reactor 2 is a fixed bed, the particle diameter of the metal-based catalyst is 0.3 to 6mm; when the primary reactor 2 is a fluidized bed, the metal-based catalyst has a particle size of 0.03 to 0.3mm.
S2, enabling the mixed gas to enter a secondary reactor 3 through pores of a porous plate 4, and enabling CO in the mixed gas and water vapor to undergo catalytic conversion under the action of a water gas catalyst to generate hydrogen, so as to finally obtain CO-free product gas;
specifically, the space velocity of the mixed gas entering the secondary reactor 3 is 1000-20000ml/gcat/h. The temperature in the secondary reactor 3 is controlled by a heat exchange device 6, and the temperature is 180-220 ℃; the water gas catalyst is an iron-based catalyst or a copper-based catalyst; and, when the secondary reactor 3 is a fixed bed, the particle diameter of the metal-based catalyst is 0.3 to 6mm; when the secondary reactor 3 is a fluidized bed, the particle size of the metal-based catalyst is 0.03 to 0.3mm.
Step S1, under the action of a metal-based catalyst, the synthesis gas reacts by a primary reactor to obtain water vapor, CO and CO 2 And in the step S2, the mixed gas is further subjected to catalytic treatment in a secondary reactor, so that CO in the mixed gas and water vapor are subjected to catalytic conversion to generate hydrogen, and CO in the product is removed. Since the product gas outlet of the secondary reactor contains little CO and water, the subsequent separation device is reduced by 33%. The investment cost is reduced by 25 percent, and the running cost is reduced by 20 percent. And because the mixed gas carries a large amount of heat energy, when entering the secondary reactor for further reaction, the heat energy is not required to be additionally provided for further conversion of water vapor and CO in the mixed gas, and the heat exchange device is used for effectively controlling the secondary reactor to supply heat for the secondary reactor by utilizing the reaction heat in the primary reactor, so that the energy saving and emission reduction targets are realized.
S3, discharging the product gas out of the secondary reactor 3 through a product gas outlet 8, and separating to obtain hydrogen and target product olefin; the hydrogen is further used for preparing synthesis gas for recycling.
The hydrogen obtained by separation in the step can be directly used for configuration of synthesis gas, so that recycling of the hydrogen is realized. Compared with the method without conversion of a secondary reactor, the method directly utilizes the hydrogen in the mixed product 1, avoids the material consumption and the energy consumption which are spent in the preparation of the hydrogen-carbon ratio, and can save the cost by 20 percent.
In some embodiments, in the synthesis gas, H 2 The volume ratio of the catalyst to CO is 1.25:1-2.5:1.
In order to make the present invention more clearly understood by those skilled in the art, a reaction apparatus and method for efficiently converting synthesis gas according to the present invention will now be described in detail by the following examples.
Example 1
The reaction device shown in FIG. 1 (the primary reactor 2 and the secondary reactor 3 are both fixed beds), an iron-based catalyst (particle size of 0.03-0.2 mm) is filled on the side of the primary reactor 2 close to the heating device 5, an iron-based catalyst (particle size of 0.5-3 mm) is filled on the side of the secondary reactor 3 close to the porous plate 4, and a copper-based catalyst (particle size of 0.5-3 mm) is filled on the side of the secondary reactor 3 close to the product gas outlet 8.
Introducing synthesis gas from a feed gas inlet 7 into the reactor at a space velocity of 1000-5000ml/gcat/H to obtain synthesis gas H 2 CO is 2:1, the temperature of the iron-based catalyst section in the primary reactor 2 is controlled to be stable at 350 ℃ by a heating device 5, and the pressure in the primary reactor 2 is 2MPa. The synthesis gas is subjected to catalytic conversion to obtain mixed gas containing olefin, wherein the carbon number of hydrocarbon is distributed to be 1-7, and the olefin selectivity is 90 percent (hydrocarbon group). The CO conversion was 96%. The mixed gas exits the primary reactor 2 from the perforated plate 4 and enters the secondary reactor 3.
In the secondary reactor 3, the space velocity of the mixed gas is 10000-20000 ml/gcat/h. The temperature of the iron-based catalyst section is controlled to 280 ℃ and the temperature of the copper-based catalyst section is controlled to 180 ℃ by controlling the flow of the heat exchange medium in the heat exchange device 6, so that H in the mixed gas 2 O and residual CO generate water gas shift reaction to generate H 2 With CO 2 . The total CO conversion was 99.9%. The product gas obtained by the clock is discharged from the outlet 8 to enter the subsequent separation process.
And (5) separating the obtained hydrogen for recycling.
Example 2
The reaction apparatus shown in FIG. 2 (fluidized beds for both the primary reactor 2 and the secondary reactor 3) was used, a cobalt-based catalyst (particle size: 0.05 to 0.25 mm) was charged on the side of the primary reactor 2 close to the heating apparatus 5, an iron-based catalyst (particle size: 0.5 to 3 mm) was charged on the side of the secondary reactor 3 close to the porous plate 4, and a copper-based catalyst (particle size: 0.05 to 0.3 mm) was charged on the side of the secondary reactor 3 close to the product gas outlet 8.
Introducing synthesis gas from a feed gas inlet 7 into the reactor at a space velocity of 5000-10000ml/gcat/H to obtain synthesis gas H 2 CO is 1.5:1, the temperature of the cobalt-based catalyst section in the primary reactor 2 is controlled to be stable at 250 ℃ by a heating device 5, and the pressure in the primary reactor 2 is 6MPa. The synthesis gas is subjected to catalytic conversion to obtain mixed gas containing olefin, wherein the carbon number of hydrocarbon is distributed to be 1-7, and the selectivity of the olefin is 85 percent (hydrocarbon group). The CO conversion was 90%. The mixed gas exits the primary reactor 2 from the perforated plate 4 and enters the secondary reactor 3.
In the secondary reactor 3, the space velocity of the mixed gas is 2000-5000ml/gcat/h. The temperature of the iron-based catalyst section is controlled to 240 ℃ and the temperature of the copper-based catalyst section is controlled to 180-200 ℃ by controlling the flow of the heat exchange medium in the heat exchange device 6, so that H in the mixed gas 2 O and residual CO generate water gas shift reaction to generate H 2 With CO 2 . The total CO conversion was 99%. The final product gas is discharged from the outlet 8 and enters the subsequent separation process.
And (5) separating the obtained hydrogen for recycling.
Example 3
The reaction apparatus shown in FIG. 3 (the primary reactor 2 is a fluidized bed, the secondary reactor 3 is a fixed bed), an iron-based catalyst (particle size 0.05-0.18 mm) is packed on the side of the primary reactor 2 near the heating apparatus 5, an iron-based catalyst (particle size 3-6 mm) is packed on the side of the secondary reactor 3 near the porous plate 4, and a copper-based catalyst (particle size 5-6 mm) is packed on the side of the secondary reactor 3 near the product gas outlet 8.
Introducing synthesis gas from a raw material gas inlet 7 into the reactor at a space velocity of 3000-6000ml/gcat/H to synthesize gas H 2 CO is 1.8:1, the primary reactor is controlled by a heating device 52, the temperature of the iron-based catalyst section in the first reactor 2 was stabilized at 325 ℃, and the pressure in the first reactor 2 was 3MPa. The synthesis gas is subjected to catalytic conversion to obtain mixed gas containing olefin, wherein the carbon number of hydrocarbon is distributed to be 1-7, and the selectivity of olefin is 88 percent (hydrocarbon group). The CO conversion was 94.5%. The mixed gas exits the primary reactor 2 from the perforated plate 4 and enters the secondary reactor 3.
In the secondary reactor 3, the space velocity of the mixed gas is 5000-10000ml/gcat/h. The temperature of the iron-based catalyst section is controlled to be 260-270 ℃ and the temperature of the copper-based catalyst section is controlled to be 200 ℃ by controlling the flow of the heat exchange medium in the heat exchange device 6, so that H in the mixed gas is generated 2 O and residual CO generate water gas shift reaction to generate H 2 With CO 2 . The total CO conversion was 99.1%. The final product gas is discharged from the outlet 8 and enters the subsequent separation process.
And (5) separating the obtained hydrogen for recycling.
Example 4
The reaction device shown in FIG. 1 (the primary reactor 2 and the secondary reactor 3 are both fixed beds), an iron-based catalyst (particle size 0.05-0.25 mm) is filled on the side of the primary reactor 2 close to the heating device 5, an iron-based catalyst (particle size 2-4 mm) is filled on the side of the secondary reactor 3 close to the porous plate 4, and a copper-based catalyst (particle size 2-6 mm) is filled on the side of the secondary reactor 3 close to the product gas outlet 8.
Introducing synthesis gas from a feed gas inlet 7 into the reactor at a space velocity of 2000-4000ml/gcat/H to obtain synthesis gas H 2 CO 1.25:1, the temperature of the iron-based catalyst section in the primary reactor 2 is controlled to be stable at 300 ℃ by a heating device 5, and the pressure in the primary reactor 2 is 4MPa. The synthesis gas is subjected to catalytic conversion to obtain mixed gas containing olefin, wherein the carbon number of hydrocarbon is distributed to be 1-7, and the olefin selectivity is 95 percent (hydrocarbon group). The CO conversion was 90%. The mixed gas exits the primary reactor 2 from the perforated plate 4 and enters the secondary reactor 3.
In the secondary reactor 3, the space velocity of the mixed gas was 3000ml/gcat/h. The temperature of the iron-based catalyst section is controlled to be 240-250 ℃ and the temperature of the copper-based catalyst section is controlled to be 180-190 ℃ by controlling the flow of the heat exchange medium in the heat exchange device 6, so that the mixture is realizedH in gas mixture 2 O and residual CO generate water gas shift reaction to generate H 2 With CO 2 . The total CO conversion was 99.5%. The final product gas is discharged from the outlet 8 and enters the subsequent separation process.
And (5) separating the obtained hydrogen for recycling.
Example 5
The reaction apparatus shown in FIG. 2 (fluidized beds are used for the primary reactor 2 and the secondary reactor 3), an iron-based catalyst (particle size 0.07-0.20 mm) is filled on the side of the primary reactor 2 close to the heating apparatus 5, an iron-based catalyst (particle size 0.05-0.3 mm) is filled on the side of the secondary reactor 3 close to the porous plate 4, and a copper-based catalyst (particle size 0.05-0.3 mm) is filled on the side of the secondary reactor 3 close to the product gas outlet 8.
Introducing synthesis gas from a feed gas inlet 7 into the reactor at a space velocity of 1000-2000ml/gcat/H to obtain synthesis gas H 2 CO is 2.5:1, the temperature of the iron-based catalyst section in the primary reactor 2 is controlled to be stable at 280 ℃ by a heating device 5, and the pressure in the primary reactor 2 is 5MPa. The synthesis gas is subjected to catalytic conversion to obtain mixed gas containing olefin, wherein the carbon number distribution of hydrocarbon is 1-7, and the olefin selectivity is 91.5 percent (hydrocarbon group). The CO conversion was 91.6%. The mixed gas exits the primary reactor 2 from the perforated plate 4 and enters the secondary reactor 3.
In the secondary reactor 3, the space velocity of the mixed gas is 18000-20000ml/gcat/h. The temperature of the iron-based catalyst section is controlled to 240 ℃ and the temperature of the copper-based catalyst section is controlled to 200-220 ℃ by controlling the flow of the heat exchange medium in the heat exchange device 6, so that H in the mixed gas is generated 2 O and residual CO generate water gas shift reaction to generate H 2 With CO 2 . The total CO conversion was 99.2%. The final product gas is discharged from the outlet 8 and enters the subsequent separation process.
And (5) separating the obtained hydrogen for recycling.
Example 6
The reaction apparatus shown in FIG. 1 (both the primary reactor 2 and the secondary reactor 3 are fixed beds), a cobalt-based catalyst (particle size 3-6 mm) is packed on the side of the primary reactor 2 close to the heating apparatus 5, an iron-based catalyst (particle size 3-6 mm) is packed on the side of the secondary reactor 3 close to the porous plate 4, and a copper-based catalyst (particle size 2-4 mm) is packed on the side of the secondary reactor 3 close to the product gas outlet 8.
Introducing synthesis gas from a feed gas inlet 7 into the reactor at a space velocity of 2000-3000ml/gcat/H to obtain synthesis gas H 2 CO is 2:1, the temperature of the cobalt-based catalyst section in the primary reactor 2 is controlled to be stable at 340 ℃ by a heating device 5, and the pressure in the primary reactor 2 is 2.6MPa. The synthesis gas is subjected to catalytic conversion to obtain mixed gas containing olefin, wherein the carbon number distribution of hydrocarbon is 1-7, and the olefin selectivity is 87.5 percent (hydrocarbon group). The CO conversion was 96%. The mixed gas exits the primary reactor 2 from the perforated plate 4 and enters the secondary reactor 3.
In the secondary reactor 3, the space velocity of the mixed gas was 1800-4600ml/gcat/h. The temperature of the iron-based catalyst section is controlled to be 240-250 ℃ and the temperature of the copper-based catalyst section is controlled to be 190-210 ℃ by controlling the flow of the heat exchange medium in the heat exchange device 6, so that H in the mixed gas is generated 2 O and residual CO generate water gas shift reaction to generate H 2 With CO 2 . The total CO conversion was 99.2%. The final product gas is discharged from the outlet 8 and enters the subsequent separation process.
And (5) separating the obtained hydrogen for recycling.
In the description of the present specification, a description referring to terms "one embodiment," "some embodiments," "examples," "specific examples," or "some examples," etc., means that a particular feature, structure, material, or characteristic described in connection with the embodiment or example is included in at least one embodiment or example of the present invention. In this specification, schematic representations of the above terms are not necessarily directed to the same embodiment or example. Furthermore, the particular features, structures, materials, or characteristics described may be combined in any suitable manner in any one or more embodiments or examples. Furthermore, one skilled in the art can combine and combine the different embodiments or examples described in this specification.
For the purposes of simplicity of explanation, the methodologies are shown as a series of acts, but one of ordinary skill in the art will recognize that the present invention is not limited by the order of acts described, as some acts may, in accordance with the present invention, occur in other orders and concurrently. Further, those skilled in the art will recognize that the embodiments described in the specification are all of the preferred embodiments, and that the acts and components referred to are not necessarily required by the present invention.
The above-mentioned reaction device and method for high-efficiency conversion of synthesis gas provided by the invention are described in detail, and specific examples are applied to illustrate the principles and embodiments of the invention, and the above examples are only used to help understand the method and core idea of the invention; meanwhile, as those skilled in the art will have variations in the specific embodiments and application scope in accordance with the ideas of the present invention, the present description should not be construed as limiting the present invention in view of the above.
Claims (10)
1. A reaction device for efficiently converting synthesis gas, which is characterized by comprising a primary reactor and a secondary reactor; the primary reactor and the secondary reactor are separated by a porous plate;
the primary reactor is used for carrying out catalytic conversion on the synthesis gas to obtain mixed gas containing olefin;
the secondary reactor is used for carrying out catalytic conversion on unreacted CO in the primary reactor and water vapor generated by the reaction to generate hydrogen, and finally obtaining CO-free product gas;
the primary reactor is provided with a heating device, and the secondary reactor is provided with a heat exchange device to realize independent temperature control.
2. The reaction apparatus of claim 1, wherein the primary reactor is configured as a fixed bed or a fluidized bed and the secondary reactor is configured as a fixed bed or a fluidized bed.
3. The reaction apparatus of claim 2, wherein the primary reactor and the secondary reactor are each configured as a fixed bed.
4. The reaction apparatus of claim 1, wherein a feed gas inlet is provided at the bottom of the primary reactor; the top of the secondary reactor is provided with a product gas outlet;
the secondary reactor is provided with two catalyst filling ports which are respectively close to the porous plate and the product gas outlet.
5. A process for the efficient conversion of synthesis gas, suitable for use in a reaction apparatus according to any one of claims 1 to 4, comprising the steps of:
s1, introducing synthesis gas into a first-stage reactor through a feed gas inlet, and reacting the synthesis gas under the action of a metal-based catalyst to obtain mixed gas containing olefin; the mixed gas comprises water vapor, CO and CO 2 And C1-C7 hydrocarbons;
s2, enabling the mixed gas to enter a secondary reactor through pores of a porous plate, and carrying out catalytic conversion on CO and steam in the mixed gas under the action of a water gas catalyst to generate hydrogen so as to obtain CO-free product gas;
s3, discharging the product gas out of the secondary reactor through a product gas outlet, and separating to obtain hydrogen and target product olefin; the hydrogen is further used for configuring the synthesis gas for recycling.
6. The method for efficient conversion of synthesis gas according to claim 5, wherein in step S1, the temperature in the primary reactor is controlled by a heating device, and the temperature is 240-280 ℃;
the metal-based catalyst is an iron-based catalyst or a cobalt-based catalyst;
when the primary reactor is a fixed bed, the particle size of the metal-based catalyst is 0.3-6mm;
when the primary reactor is a fluidized bed, the particle size of the metal-based catalyst is 0.03-0.3mm.
7. The method for efficient conversion of synthesis gas according to claim 5, wherein in step S2, the temperature in the secondary reactor is controlled by a heat exchange device, and the temperature is 180-220 ℃;
the water gas catalyst is an iron-based catalyst or a copper-based catalyst;
when the secondary reactor is a fixed bed, the particle size of the metal-based catalyst is 0.3-6mm;
when the secondary reactor is a fluidized bed, the particle size of the metal-based catalyst is 0.03-0.3mm.
8. The method for efficient conversion of synthesis gas according to claim 5, wherein in step S1, the space velocity of the synthesis gas ranges from 1000 to 10000ml/gcat/h.
9. The method for efficient conversion of synthesis gas according to claim 5, wherein in step S2, the space velocity of the mixed product 1 in the secondary reactor is 1000-20000ml/gcat/h.
10. The method for efficient conversion of synthesis gas according to claim 5, wherein H in the synthesis gas 2 The volume ratio of the catalyst to CO is 1.25:1-2.5:1.
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