CN116637561A - Trickle bed reactor and method for preparing m-xylylenediamine by using same - Google Patents
Trickle bed reactor and method for preparing m-xylylenediamine by using same Download PDFInfo
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- CN116637561A CN116637561A CN202310630258.9A CN202310630258A CN116637561A CN 116637561 A CN116637561 A CN 116637561A CN 202310630258 A CN202310630258 A CN 202310630258A CN 116637561 A CN116637561 A CN 116637561A
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- FDLQZKYLHJJBHD-UHFFFAOYSA-N [3-(aminomethyl)phenyl]methanamine Chemical compound NCC1=CC=CC(CN)=C1 FDLQZKYLHJJBHD-UHFFFAOYSA-N 0.000 title claims abstract description 52
- 238000000034 method Methods 0.000 title claims abstract description 33
- 239000007788 liquid Substances 0.000 claims abstract description 88
- 239000003054 catalyst Substances 0.000 claims abstract description 67
- 239000000945 filler Substances 0.000 claims abstract description 21
- 238000012856 packing Methods 0.000 claims abstract description 16
- 239000007789 gas Substances 0.000 claims description 27
- 230000008602 contraction Effects 0.000 claims description 23
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 19
- 238000009903 catalytic hydrogenation reaction Methods 0.000 claims description 18
- 238000006243 chemical reaction Methods 0.000 claims description 18
- LAQPNDIUHRHNCV-UHFFFAOYSA-N isophthalonitrile Chemical compound N#CC1=CC=CC(C#N)=C1 LAQPNDIUHRHNCV-UHFFFAOYSA-N 0.000 claims description 15
- 239000002904 solvent Substances 0.000 claims description 13
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 claims description 12
- 239000001257 hydrogen Substances 0.000 claims description 12
- 229910052739 hydrogen Inorganic materials 0.000 claims description 12
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 11
- 229910052759 nickel Inorganic materials 0.000 claims description 10
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 9
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 claims description 9
- 239000002131 composite material Substances 0.000 claims description 9
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 6
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 claims description 6
- XDTMQSROBMDMFD-UHFFFAOYSA-N Cyclohexane Chemical compound C1CCCCC1 XDTMQSROBMDMFD-UHFFFAOYSA-N 0.000 claims description 3
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 claims description 3
- 150000001875 compounds Chemical class 0.000 claims 1
- 238000012546 transfer Methods 0.000 abstract description 15
- 239000012071 phase Substances 0.000 abstract description 12
- 239000007791 liquid phase Substances 0.000 abstract description 8
- 238000010812 external standard method Methods 0.000 description 14
- 238000004811 liquid chromatography Methods 0.000 description 14
- 238000004458 analytical method Methods 0.000 description 12
- 230000000052 comparative effect Effects 0.000 description 9
- 238000009826 distribution Methods 0.000 description 7
- 238000012360 testing method Methods 0.000 description 7
- 239000007787 solid Substances 0.000 description 5
- 238000009736 wetting Methods 0.000 description 5
- 230000009471 action Effects 0.000 description 4
- 230000001154 acute effect Effects 0.000 description 4
- 239000004973 liquid crystal related substance Substances 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 230000008859 change Effects 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000002474 experimental method Methods 0.000 description 3
- 239000012530 fluid Substances 0.000 description 3
- 238000012986 modification Methods 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- 239000004033 plastic Substances 0.000 description 3
- 229920003023 plastic Polymers 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 2
- 230000006978 adaptation Effects 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- 230000005465 channeling Effects 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- 150000002431 hydrogen Chemical class 0.000 description 2
- QZUPTXGVPYNUIT-UHFFFAOYSA-N isophthalamide Chemical compound NC(=O)C1=CC=CC(C(N)=O)=C1 QZUPTXGVPYNUIT-UHFFFAOYSA-N 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 150000002739 metals Chemical class 0.000 description 2
- 229920006391 phthalonitrile polymer Polymers 0.000 description 2
- 238000011112 process operation Methods 0.000 description 2
- 230000010349 pulsation Effects 0.000 description 2
- 239000007790 solid phase Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 230000005514 two-phase flow Effects 0.000 description 2
- 239000004677 Nylon Substances 0.000 description 1
- 238000004220 aggregation Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 238000001311 chemical methods and process Methods 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 238000006757 chemical reactions by type Methods 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000004581 coalescence Methods 0.000 description 1
- 230000009849 deactivation Effects 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 229920001971 elastomer Polymers 0.000 description 1
- 239000003822 epoxy resin Substances 0.000 description 1
- 239000012847 fine chemical Substances 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000011031 large-scale manufacturing process Methods 0.000 description 1
- 239000000314 lubricant Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 229920001778 nylon Polymers 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 238000013021 overheating Methods 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 238000005504 petroleum refining Methods 0.000 description 1
- 238000011020 pilot scale process Methods 0.000 description 1
- 229920000647 polyepoxide Polymers 0.000 description 1
- 229920005749 polyurethane resin Polymers 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 239000011949 solid catalyst Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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
- B01J8/02—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
- B01J8/0446—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 the flow within the beds being predominantly vertical
- B01J8/0449—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 the flow within the beds being predominantly vertical in two or more cylindrical beds
- B01J8/0453—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 the flow within the beds being predominantly vertical in two or more cylindrical beds the beds being superimposed one above the other
-
- 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
- B01J8/0492—Feeding reactive fluids
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C209/00—Preparation of compounds containing amino groups bound to a carbon skeleton
- C07C209/44—Preparation of compounds containing amino groups bound to a carbon skeleton by reduction of carboxylic acids or esters thereof in presence of ammonia or amines, or by reduction of nitriles, carboxylic acid amides, imines or imino-ethers
- C07C209/48—Preparation of compounds containing amino groups bound to a carbon skeleton by reduction of carboxylic acids or esters thereof in presence of ammonia or amines, or by reduction of nitriles, carboxylic acid amides, imines or imino-ethers by reduction of nitriles
-
- 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
- Y02P20/584—Recycling of catalysts
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Abstract
A trickle bed reactor comprises a reactor shell, wherein a liquid distributor, at least one liquid redistributor and at least one layer of supporting plate are sequentially arranged in the reactor shell at intervals from top to bottom, and the inside of the reactor shell is sequentially divided into a gas cavity, at least 2 catalyst beds and a liquid cavity from top to bottom; the catalyst bed layer is filled with a three-dimensional pulse filler; the top of the device is provided with a gas phase inlet, the bottom of the device is provided with a liquid outlet, and the side wall of the device is provided with a liquid inlet and a gas outlet at positions corresponding to the liquid distributor and the liquid cavity; the three-dimensional pulse packing comprises a three-dimensional pulse tube bundle vertically arranged in the catalyst bed layer, the three-dimensional pulse tube bundle comprises a plurality of three-dimensional pulse tubes which are arranged in parallel and in a dispersed manner, the three-dimensional pulse tubes are provided with vertical first liquid channels, and vertical second liquid channels are formed between adjacent three-dimensional pulse tubes. Also provided are methods of producing m-xylylenediamine using the foregoing trickle bed reactors. The trickle bed reactor can improve the turbulence degree and mass transfer efficiency of gas and liquid phases in a bed.
Description
Technical Field
The invention belongs to the technical field of equipment and production, and particularly relates to a trickle bed reactor and a method for preparing m-xylylenediamine by using the trickle bed reactor.
Background
The trickle bed reactor is a typical gas-liquid-solid three-phase reactor, can obtain higher conversion rate, is widely applied to chemical processes such as petroleum refining, petrochemical industry, fine chemical industry and the like, and is mainly applied to reaction types such as hydrogenation, oxidation and the like. Trickle bed reactors, however, also suffer from the following disadvantages: in pilot experiments, the radial distribution of liquid flow operated at low liquid velocity is uneven, which may cause incomplete wetting of the solid catalyst, uneven temperature distribution, hot spot formation, rapid deactivation of the catalyst or influence on the gas-liquid flow state, which are unfavorable for the operation of trickle bed reactor. Therefore, there is a need for an improvement in trickle bed reactors to achieve operation at the boundary of the trickle flow region and the pulse flow region as much as possible, to provide a relatively uniform gas-liquid phase distribution, and to avoid localized overheating.
The m-xylylenediamine is colorless liquid, is dissolved in water and organic solvent, is mainly used for preparing heat-resistant and fast-curing high-performance epoxy resin curing agent, is a raw material of polyurethane resin, and also has application in the fields of rubber products, photosensitive plastics, nylon products, lubricants and the like. The current synthetic route of m-xylylenediamine is mainly batch method synthesis, large-scale production cannot be carried out, while the continuous chemical route is mainly carried out in a trickle bed reactor, but the gas-liquid two-phase flow rate in a small test experiment is low, and the gas-liquid two-phase flow rate is in a trickle zone, so that accurate valuable data cannot be provided for pilot-scale or industrial reactors. Therefore, aiming at the problems of the existing small-scale continuous test at present, an improved trickle bed reactor is required to be sought so as to improve the turbulence degree of gas-liquid two phases in small-scale test, strengthen mass and heat transfer and provide accurate data for the operation of an industrial reactor.
Disclosure of Invention
A first object of the present invention is to provide a trickle bed reactor with a three-dimensional pulse packing which can improve the turbulence degree and mass transfer efficiency of the gas and liquid phases in the bed, and is suitable for catalytic hydrogenation reaction;
the second object of the present invention is to provide a method for preparing m-xylylenediamine using the trickle bed reactor, which is simple and easy to operate, and enhances mass transfer and heat transfer between three phases of gas, liquid and solid, thereby improving the data accuracy of pilot experiments.
In order to achieve the first object of the present invention, the following technical solutions are adopted:
a trickle bed reactor comprising a reactor shell;
the reactor comprises a reactor shell, a liquid distributor, at least one liquid redistributor and at least one layer of supporting plate, wherein the reactor shell is internally provided with the liquid distributor, the at least one liquid redistributor and the at least one layer of supporting plate at intervals from top to bottom, and the reactor shell is internally divided into a gas cavity, at least 2 catalyst beds and a liquid cavity from top to bottom in sequence; the catalyst bed layer is filled with a three-dimensional pulse filler;
the top of the reactor shell is provided with a gas phase inlet, the bottom of the reactor shell is provided with a liquid outlet, the side wall of the reactor shell is provided with a liquid inlet corresponding to the liquid distributor, and the side wall of the reactor shell is provided with a gas outlet corresponding to the liquid cavity;
the three-dimensional pulse packing comprises a three-dimensional pulse tube bundle vertically arranged in the catalyst bed layer, wherein the three-dimensional pulse tube bundle comprises a plurality of three-dimensional pulse tubes which are arranged in parallel and in a dispersed manner, each three-dimensional pulse tube is provided with a first vertical liquid channel, and a second vertical liquid channel is formed between every two adjacent three-dimensional pulse tubes.
In the trickle bed reactor of the present invention, preferably, the stereoscopic pulse tube includes a contraction section and an expansion section alternately arranged along a length direction thereof, and adjacent contraction section and expansion section form one pulse unit; the stereoscopic pulse tube comprises 50-200 pulse units;
preferably, the area of the largest cross section in the pulse unit is 10-50mm 2 The method comprises the steps of carrying out a first treatment on the surface of the And/or
The area ratio of the smallest cross section to the largest cross section in the pulse unit is 0.01-0.25.
The trickle bed reactor of the present invention, preferably, the length ratio of the expansion section to the contraction section is 1/3-1; and/or
The ratio of the specific surface area of the expansion section to the specific surface area of the contraction section is 1-3.
The trickle bed reactor of the present invention, preferably, the length of the constriction is 5-15mm; and/or
The specific surface area of the contraction section is 1-5m 2 /m 3 。
In the trickle bed reactor of the present invention, preferably, in the three-dimensional pulse packing, the three-dimensional pulse tube bundles are arranged within the catalyst bed in the following manner: adjacent 3 three-dimensional pulse tubes are arranged in a regular triangle, so that a minimum arrangement unit is formed;
preferably, in the minimum arrangement unit, the arrangement directions of adjacent 2 of the stereoscopic pulse tubes differ by 120 °;
preferably, the distance between two adjacent 2 solid pulse tubes is L1 according to the distance between the vertical central axes of the two solid pulse tubes, and the length of the longest side of the largest cross section in the pulse unit is L2, then L1/l2=0.5-5.
The trickle bed reactor of the present invention, preferably,
the material of the three-dimensional pulse filler is any one or a combination of a plurality of plastics, metals, ceramics or glass; and/or
The height-diameter ratio of the catalyst bed layer is 3-8; and/or
The liquid redistributor is of a truncated cone structure.
To achieve the second object of the present invention, there is also provided a method for preparing m-xylylenediamine using the trickle bed reactor as described above, the method comprising:
(1) Introducing hydrogen into the trickle bed reactor from the gas phase inlet to activate the catalyst filled in the catalyst bed;
(2) Introducing a composite solvent dissolved with isophthalonitrile into the trickle bed reactor from the liquid inlet, carrying out catalytic hydrogenation reaction on the catalyst bed layer and the introduced hydrogen to prepare m-xylylenediamine, and outputting the m-xylylenediamine from the liquid outlet.
In one embodiment, the method, the trickle bed reactor, the three-dimensional pulse filling (5) has a pulse frequency of 0.01-10s -1 。
In one embodiment, the catalyst packed in the catalyst bed is a nickel-based catalyst;
preferably, the nickel-based catalyst is a framework-type catalyst or a supported catalyst, and the nickel content is more than or equal to 5wt%.
In one embodiment, the complex solvent comprises a combination of any two or more of tetrahydrofuran, methanol, toluene, cyclohexane, liquid ammonia, N-methylpyrrolidone; and/or
In the catalytic hydrogenation reaction, the molar ratio of isophthalonitrile to hydrogen to composite solvent is 1 (1-10) (2-40); and/or
In the catalytic hydrogenation reaction, the reaction pressure is 6-20MPa, and/or the reaction temperature is 50-100 ℃.
The invention has the beneficial effects that:
(1) The trickle bed reactor is internally provided with the three-dimensional pulse filler, and the special pulse characteristic of the three-dimensional pulse filler can greatly improve the wetting degree of the catalyst, so that 'pulsation' is generated in the bed layer, and the turbulence degree and mass transfer efficiency of gas and liquid phases in the bed layer can be improved;
(2) According to the trickle bed reactor, the liquid redistributors are arranged between the adjacent catalyst beds, and the special structure of the liquid redistributors enables liquid to be dispersed again, so that channeling of the liquid and aggregation of gas are reduced, the contact area of gas and liquid is increased, and the gas-liquid mass transfer efficiency is improved;
(3) The trickle bed reactor can strengthen heat transfer and mass transfer among gas, liquid and solid under the combined action of the three-dimensional pulse filler and the liquid redistributor, so that the flow pattern in the bed is close to the adjacent areas of trickle flow and pulse flow, the flow pattern is more stable, and the phenomenon of uneven temperature and concentration distribution can be avoided; the catalyst is suitable for catalytic hydrogenation reaction;
(4) The method for preparing the m-xylylenediamine by utilizing the trickle bed reactor is simple and easy to operate, greatly improves the wetting degree of the catalyst under the combined action of the three-dimensional pulse filler and the liquid redistributor, ensures that the flow pattern in the bed layer is close to the adjacent areas of the trickle flow and the pulse flow, is more stable, avoids the phenomenon of uneven temperature and concentration distribution, can improve the airspeed of a small test device, improves the data accuracy of the small test device, and provides more accurate data for an industrial device; and simultaneously, the process operation condition is reduced.
Drawings
FIG. 1 is a schematic diagram of the trickle bed reactor of the present invention in one embodiment;
FIG. 2 is a schematic diagram of the pulsing unit of the stereoscopic pulsing packing in the trickle bed reactor of the present invention in one embodiment;
fig. 3 is a schematic diagram of the arrangement of a stereoscopic pulse tube (also a schematic cross-sectional structure thereof) of a stereoscopic pulse packing in a trickle bed reactor according to the present invention in one embodiment.
Detailed Description
The technical scheme and effects of the present invention are further described below with reference to the detailed description/examples and the accompanying drawings. The following embodiments/examples are only for illustrating the contents of the present invention, and the present invention is not limited to the following embodiments or examples. Simple modifications of the invention using the inventive concept are within the scope of the invention as claimed.
The present invention provides a trickle bed reactor, as shown in figures 1-3, comprising a reactor housing 10;
the reactor shell 10 is internally provided with a liquid distributor 2, at least one liquid redistributor 6 and at least one layer of supporting plate 7 at intervals from top to bottom in sequence, and the reactor shell is internally divided into a gas cavity, at least 2 catalyst beds 4 and a liquid cavity from top to bottom in sequence; the catalyst bed layer 4 is filled with a three-dimensional pulse filler 5;
the top of the reactor shell 10 is provided with a gas phase inlet 1, the bottom is provided with a liquid outlet 9, the side wall of the reactor shell is provided with a liquid inlet 3 corresponding to the liquid distributor 2, and the side wall of the reactor shell is provided with a gas outlet 8 corresponding to the liquid cavity;
the three-dimensional pulse packing 5 comprises a three-dimensional pulse tube bundle vertically arranged in the catalyst bed layer 4, the three-dimensional pulse tube bundle comprises a plurality of three-dimensional pulse tubes 51 which are arranged in parallel and in a dispersed mode, the three-dimensional pulse tubes 51 are provided with vertical first liquid channels, and vertical second liquid channels are formed between adjacent three-dimensional pulse tubes 51.
The trickle bed reactor is internally provided with the three-dimensional pulse filler, and the special pulse characteristic of the three-dimensional pulse filler can greatly improve the wetting degree of the catalyst, so that 'pulsation' is generated in the bed layer, and the turbulence degree and mass transfer efficiency of gas and liquid phases in the bed layer can be improved; the liquid redistributors are arranged between the adjacent catalyst beds, and the special structure of the liquid redistributors enables liquid to be dispersed again, so that channeling of the liquid and coalescence of gas are reduced, the contact area of gas and liquid is increased, and the gas-liquid mass transfer efficiency is improved; under the combined action of the three-dimensional pulse filler and the liquid redistributor, the heat transfer and mass transfer among the gas phase, the liquid phase and the solid phase can be enhanced, so that the flow pattern in the bed layer is close to the adjacent areas of the trickle flow and the pulse flow, the flow pattern is more stable, and the phenomenon of uneven temperature and concentration distribution can be avoided; is suitable for catalytic hydrogenation reaction.
In one embodiment, the stereoscopic pulse tube 51 includes convergent sections 511 and divergent sections 512 alternately arranged along a length direction thereof, and adjacent convergent sections 511 and divergent sections 512 form one pulse unit; the stereoscopic pulse tube 51 includes 50-200 pulse units, such as 60, 70, 80, 90, 100, 110, 120, 130, 140, 150, 160, 170, 180, and 190.
In the present invention, the constricted section 511 means a portion of which the cross-sectional area decreases in order from top to bottom, and the expanded section 512 means a portion of which the cross-sectional area increases in order from top to bottom.
In one embodiment, the area of the largest cross section in the pulse unit is 10-50mm 2 Such as 15mm 2 、20mm 2 、25mm 2 、30mm 2 、35mm 2 、40mm 2 And 45mm 2 。
In one embodiment, the area ratio of the smallest cross section to the largest cross section in the pulse unit is 0.01-0.25, such as 0.03, 0.05, 0.07, 0.1, 0.13, 0.15, 0.17, 0.2, 0.22, and 0.24, effective to form a pulse.
In one embodiment, the length ratio of the expansion section 512 to the contraction section 511 is 1/3-1, such as 1/3, 3/8, 1/2, 5/8, 2/3, 3/4, 7/8, and 1; preferably less than 1 on this basis.
In the present invention, the lengths of the expansion section 512 and the contraction section 511 refer to the lengths of both along the length direction of the stereoscopic pulse tube 51, respectively.
In the present invention, as the length of the expansion section 512 is smaller, the rate of change of the velocity of the fluid in the expansion section 512 is larger, thereby improving the impulse effect.
In one embodiment, the ratio of the specific surface area of the expansion section 512 to the contraction section 511 is 1-3, such as 1.1, 1.2, 1.3, 1.4, 1.5, 1.6, 1.7, 1.8, 1.9, 2, 2.1, 2.2, 2.3, 2.4, 2.5, 2.6, 2.7, 2.8, and 2.9; preferably greater than 1 on this basis, to enable the fluid to change at a faster rate in the expansion section 512, thereby effectively forming a pulse.
In the present invention, the specific surface area of the expansion section 512 refers to the surface area of the volume-based pulse filler.
Those skilled in the art understand that the volume is inversely proportional to the specific surface area, the larger the volume, the smaller the specific surface area, and conversely, the smaller the volume, the larger the specific surface area. The ratio of the specific surface area of the expansion section 512 to the specific surface area of the contraction section 511 is 1-3, which indicates that the specific surface area of the expansion section 512 is greater than or equal to the specific surface area of the contraction section 511, and correspondingly, the volume of the expansion section 512 is less than or equal to the volume of the contraction section 511, so that the speed change rate of the fluid in the expansion section 512 is larger, and a pulse is effectively formed.
In one embodiment, the length of the constriction 511 is 5-15mm, such as 6mm, 7mm, 8mm, 9mm, 10mm, 11mm, 12mm, 13mm, and 14mm.
In one embodiment, the constriction 511 has a specific surface area of 1-5m 2 /m 3 Such as 1.5m 2 /m 3 、2m 2 /m 3 、2.5m 2 /m 3 、3m 2 /m 3 、3.5m 2 /m 3 、4m 2 /m 3 And 4.5m 2 /m 3 。
The cross section of the pulse unit can be in any form, so as to improve the pulse effect and further improve the heat transfer and mass transfer between the gas phase, the liquid phase and the solid phase, and in one embodiment, the cross section of the pulse unit is polygonal, preferably triangular, and further preferably acute triangular.
In one embodiment, the three included angles of the acute triangle are 40-60 °, such as 45 °, 50 ° and 55 °, respectively; 50-70 °, such as 55 °, 60 °, and 65 °;60-90, such as 65 °, 70 °, 75 °, 80 °, and 85 °.
In one embodiment, in the stereopulse packing 5, the bundles of stereopulse tubes are arranged within the catalyst bed 4 in the following manner: adjacent 3 of the three-dimensional pulse tubes 51 are arranged in a regular triangle, forming a minimum arrangement unit.
In one embodiment, the smallest placement unit, the placement directions of adjacent 2 of the stereoscopic pulse tubes 51 differ by 120 °.
The arrangement directions of adjacent 2 of the three-dimensional pulse tubes 51 differ by 120 ° means that, in a minimum arrangement unit arranged in a regular triangle, a point where a first angle on 1 of the cross sections of a first one of the three-dimensional pulse tubes 51 is a, a point where a second angle adjacent thereto is B, and the directions of a to B are 0 ° directions (also 360 ° directions), and the directions corresponding to a to B are 120 ° directions (or-120 ° directions) in the second one of the three-dimensional pulse tubes 51 adjacent to the first one of the three-dimensional pulse tubes 51; similarly, in a third one of the stereoscopic pulse tubes 51 adjacent to a second one of the stereoscopic pulse tubes 51, the direction corresponding to a to B is 240 ° direction (or-240 ° direction). Corresponding to the smallest arrangement unit in a regular triangle arrangement, where the second one of the stereoscopic pulse tubes 51 is rotated 120 deg. clockwise/counterclockwise about its own vertical central axis and the third one of the stereoscopic pulse tubes 51 is rotated 2 times 120 deg. clockwise/counterclockwise about its own vertical central axis, compared to the arrangement direction of the first one of the stereoscopic pulse tubes 51. The arrangement directions between every two are different by 120 degrees.
In one embodiment, the distance between adjacent 2 of the stereoscopic pulse tubes 51 is L1 in terms of the distance between the vertical central axes of the two, and the length of the longest side of the largest cross section in the pulse unit is L2, then L1/l2=0.5-5, such as 1, 1.5, 2, 2.5, 3, 3.5, 4, and 4.5.
In one embodiment, the material of the three-dimensional pulse filler 5 is any one or a combination of a plurality of plastics, metals, ceramics or glass.
In one embodiment, the aspect ratio of the catalyst bed 4 is 3 to 8, such as 4, 5, 6, and 7.
In one embodiment, the liquid redistributor 6 is of a truncated cone configuration.
The present invention also provides a method for preparing m-xylylenediamine using the trickle bed reactor described above, the method comprising:
(1) Introducing hydrogen into the trickle bed reactor from the gas phase inlet 1 to activate the catalyst filled in the catalyst bed 4;
(2) Introducing a composite solvent dissolved with isophthalonitrile into the trickle bed reactor from the liquid inlet 3, carrying out catalytic hydrogenation reaction on the catalyst bed 4 and the introduced hydrogen to prepare m-xylylenediamine, and outputting the m-xylylenediamine from the liquid outlet 9.
In one embodiment, the method, the trickle bed reactor, the three-dimensional pulse filling 5 has a pulse frequency of 0.01-10s -1 Such as 0.02s -1 、0.05s -1 、0.1s -1 、0.15s -1 、0.2s -1 、0.5s -1 、1s -1 、1.5s -1 、2s -1 、2.5s -1 、3s -1 、3.5s -1 、4s -1 、4.5s -1 、5s -1 、5.5s -1 、6s -1 、6.5s -1 、7s -1 、7.5s -1 、8s -1 、8.5s -1 、9s -1 And 9.5s -1 。
In one embodiment, the catalyst packed in the catalyst bed 4 is a nickel-based catalyst.
In one embodiment, the nickel-based catalyst is a skeletal-type catalyst or a supported catalyst, and wherein the nickel content is greater than or equal to 5wt%, such as 5.5wt%, 6wt%, 5.5wt%, 7wt%, 7.5wt%, and 8wt%.
In one embodiment, the complex solvent comprises a combination of any two or more of tetrahydrofuran, methanol, toluene, cyclohexane, liquid ammonia, N-methylpyrrolidone.
In one embodiment, the molar ratio of isophthalonitrile, hydrogen, and complex solvent in the catalytic hydrogenation reaction is 1 (1-10, such as 2, 3, 4, 5, 6, 7, 8, and 9): 2-40, such as 3, 5, 10, 15, 20, 25, 30, and 35.
In one embodiment, the catalytic hydrogenation reaction is carried out at a reaction pressure of 6 to 20MPa, such as 8MPa, 10MPa, 12MPa, 14MPa, 16MPa, and 18MPa; and/or the reaction temperature is 50-100deg.C, such as 55deg.C, 60deg.C, 65deg.C, 70deg.C, 75deg.C, 80deg.C, 85deg.C, 90deg.C and 95deg.C.
The method for preparing the m-xylylenediamine by utilizing the trickle bed reactor is simple and easy to operate, greatly improves the wetting degree of the catalyst under the combined action of the three-dimensional pulse filler and the liquid redistributor, ensures that the flow pattern in the bed layer is close to the adjacent areas of the trickle flow and the pulse flow, is more stable, avoids the phenomenon of uneven temperature and concentration distribution, can improve the airspeed of a small test device, improves the data accuracy of the small test device, and provides more accurate data for an industrial device; and simultaneously, the process operation condition is reduced.
Raw material sources of raw materials used in the following examples/comparative examples:
m-phthalonitrile, >99.99%, TCI reagent limited;
tetrahydrofuran, >99.99%, available from the chemical industry, inc., of Wellling;
liquid ammonia, >99.999%, liquefied air (Shanghai) compressed gas Co., ltd;
hydrogen, 99.999%, new energy for smokestack torches limited;
catalyst, 10% Ni/supported Al 2 O 3 The catalyst is used for quick Kai catalysis.
Test methods/criteria:
the conversion rate of isophthalonitrile is analyzed by adopting a liquid chromatography external standard method; wherein, the liquid crystal display device comprises a liquid crystal display device,
conversion of isophthalonitrile= (molar amount of isophthalonitrile converted)/(molar amount of isophthalonitrile charged) ×100%;
molar yield of m-xylylenediamine is analyzed by adopting a liquid chromatography external standard method; wherein, the liquid crystal display device comprises a liquid crystal display device,
molar yield of m-xylylenediamine= (molar amount of m-xylylenediamine obtained)/(molar amount of m-xylylenediamine charged) ×100%.
Example 1 (S1)
As shown in fig. 1-3, a trickle bed reactor A1 includes a reactor housing 10;
the reactor shell 10 is internally provided with a liquid distributor 2, 2 liquid redistributors 6 and a layer of supporting plate 7 at intervals from top to bottom in sequence, and is internally divided into a gas cavity, 3 catalyst beds 4 and a liquid cavity from top to bottom in sequence; the catalyst bed layer 4 is filled with a three-dimensional pulse filler 5;
the top of the reactor shell 10 is provided with a gas phase inlet 1, the bottom is provided with a liquid outlet 9, the side wall of the reactor shell is provided with a liquid inlet 3 corresponding to the liquid distributor 2, and the side wall of the reactor shell is provided with a gas outlet 8 corresponding to the liquid cavity;
the three-dimensional pulse packing 5 comprises a three-dimensional pulse tube bundle vertically arranged in the catalyst bed layer 4, wherein the three-dimensional pulse tube bundle comprises a plurality of three-dimensional pulse tubes 51 which are arranged in parallel and in a dispersed manner, the three-dimensional pulse tubes 51 are provided with vertical first liquid channels, and vertical second liquid channels are formed between adjacent three-dimensional pulse tubes 51;
the stereoscopic pulse tube 51 includes convergent sections 511 and divergent sections 512 alternately arranged along a length direction thereof, and adjacent convergent sections 511 and divergent sections 512 form one pulse unit; the stereoscopic pulse tube 51 includes 100 pulse units;
the area of the largest cross section in the pulse unit is 25mm 2 ；
The area ratio of the minimum cross section to the maximum cross section in the pulse unit is 0.09;
the length ratio of the expansion section 512 to the contraction section 511 is 2/3;
the ratio of the specific surface area of the expansion section 512 to the contraction section 511 is 1.1.
The length of the constriction 511 is 9mm;
the specific surface area of the constriction 511 is 1.6m 2 /m 3 ；
The cross section of the pulse unit is in a regular triangle shape.
In the three-dimensional pulse packing 5, the three-dimensional pulse tube bundles are arranged within the catalyst bed 4 in the following manner: adjacent 3 of the three-dimensional pulse tubes 51 are arranged in a regular triangle to form a minimum arrangement unit;
in the minimum arrangement unit, the arrangement directions of adjacent 2 of the stereoscopic pulse tubes 51 differ by 120 °;
the distance between two adjacent 2 stereo pulse tubes 51 is L1 according to the distance between the vertical central axes of the two stereo pulse tubes, and the length of the longest side of the largest cross section in the pulse unit is L2, then L1/l2=1.5;
the material of the three-dimensional pulse filler 5 is stainless steel;
the height-diameter ratio of the catalyst bed layer 4 is 5, and the diameter is 30mm;
the liquid redistributor 6 is of a truncated cone type structure.
The preparation of m-xylylenediamine B1 using the trickle bed reactor A1 comprises:
(1) Introducing hydrogen into the trickle bed reactor from the gas phase inlet 1 to activate the catalyst filled in the catalyst bed 4;
(2) Introducing a composite solvent dissolved with isophthalonitrile into the trickle bed reactor from the liquid inlet 3, carrying out catalytic hydrogenation reaction on the catalyst bed 4 and the introduced hydrogen to prepare m-xylylenediamine B1, and outputting from the liquid outlet 9;
wherein the catalyst filled in the catalyst bed layer 4 is 10% Ni/supported Al 2 O 3 A catalyst;
the composite solvent is a composite solvent of tetrahydrofuran and liquid ammonia, and the mass ratio of the tetrahydrofuran to the liquid ammonia is 2:1;
in the catalytic hydrogenation reaction, the molar ratio of isophthalonitrile to hydrogen to composite solvent is 1:5:20;
in the catalytic hydrogenation reaction, the reaction pressure is 6MPa, and the reaction temperature is 70 ℃.
The m-xylylenediamine B1 from the liquid outlet 9 was analyzed by the liquid chromatography external standard method, and the analysis results are shown in Table 1.
Example 2 (S2)
A trickle bed reactor A2 which differs from the trickle bed reactor A1 described in example 1 only in that:
the stereoscopic pulse tube 51 includes 50 pulse units;
the area of the largest cross section in the pulse unit is 11mm 2 ；
The area ratio of the minimum cross section to the maximum cross section in the pulse unit is 0.01;
the length ratio of the expansion section 512 to the contraction section 511 is 1/3;
the ratio of the specific surface area of the expansion section 512 to the contraction section 511 is 1.4.
The length of the constriction 511 is 6mm;
the specific surface area of the constriction 511 is 2.5m 2 /m 3 。
M-xylylenediamine B2 was produced by the method of example 1 using the trickle bed reactor A2 described above.
The obtained m-xylylenediamine B2 was analyzed by the liquid chromatography external standard method, and the analysis results are shown in Table 1.
Example 3 (S3)
A trickle bed reactor A3 which differs from the trickle bed reactor A1 described in example 1 only in that:
the stereoscopic pulse tube 51 includes 200 pulse units;
the area of the largest cross section in the pulse unit is 48mm 2 ；
The area ratio of the minimum cross section to the maximum cross section in the pulse unit is 0.25;
the length ratio of the expansion section 512 to the contraction section 511 is 1;
the ratio of the specific surface area of the expansion section 512 to the contraction section 511 is 1.
The length of the constriction 511 is 13mm;
the specific surface area of the constriction 511 is 1m 2 /m 3 ；
M-xylylenediamine B3 was produced by the method of example 1 using the trickle bed reactor A3 described above; and differs from embodiment 1 only in that:
the obtained m-xylylenediamine B3 was analyzed by the liquid chromatography external standard method, and the analysis results are shown in Table 1.
Example 4 (S4)
A trickle bed reactor A4 which differs from the trickle bed reactor A1 described in example 1 only in that:
the cross section of the pulse unit is an acute triangle; the angles of the three included angles of the acute triangle are respectively 50 degrees, 60 degrees and 70 degrees;
L1/L2＝2。
m-xylylenediamine B4 was produced by the method of example 1 using the trickle bed reactor A4 described above.
The obtained m-xylylenediamine B4 was analyzed by the liquid chromatography external standard method, and the analysis results are shown in Table 1.
Example 5 (S5)
M-xylylenediamine B5 was produced by the method of example 1 using the trickle bed reactor A1; and differs from embodiment 1 only in that:
the pulse frequency of the three-dimensional pulse filler 5 is 2s -1 ；
In the catalytic hydrogenation reaction, the reaction pressure is 8MPa, and the reaction temperature is 80 ℃.
The obtained m-xylylenediamine B5 was analyzed by the liquid chromatography external standard method, and the analysis results are shown in Table 1.
Example 6 (S6)
A trickle bed reactor A6 which differs from the trickle bed reactor A1 described in example 1 only in that:
the cross section of the pulse unit is a right triangle, and the angles of the three included angles are 30 degrees, 60 degrees and 90 degrees respectively;
L1/L2＝2。
m-xylylenediamine B6 was produced by the method of example 1 using the trickle bed reactor A6 described above.
The obtained m-xylylenediamine B6 was analyzed by the liquid chromatography external standard method, and the analysis results are shown in Table 1.
Example 7 (D7)
A trickle bed reactor A7 differing from the trickle bed reactor A1 described in example 1 only in that:
the area of the largest cross section in the pulse unit is 75mm 2 ；
The area ratio of the minimum cross section to the maximum cross section in the pulse unit is 0.36;
the specific surface area of the constriction 511 is 0.8m 2 /m 3 。
M-xylylenediamine B7 was produced by the method of example 1 using the trickle bed reactor A7 described above.
The obtained m-xylylenediamine B7 was analyzed by the liquid chromatography external standard method, and the analysis results are shown in Table 1.
Example 8 (S8)
A trickle bed reactor A8 differing from the trickle bed reactor A1 described in example 1 only in that:
the cross section of the pulse unit is square.
M-xylylenediamine B8 was produced by the method of example 1 using the trickle bed reactor A8 described above.
The obtained m-xylylenediamine B8 was analyzed by the liquid chromatography external standard method, and the analysis results are shown in Table 1.
Comparative example 1 (D1)
A trickle bed reactor A1', which differs from the trickle bed reactor A1 described in example 1 only in that:
the catalyst bed layer 4 is not filled with the three-dimensional pulse packing 5.
M-xylylenediamine B1 'was produced by the method of example 1 using the trickle bed reactor A1'.
The obtained m-xylylenediamine B1' was analyzed by the liquid chromatography external standard method, and the analysis results are shown in Table 1.
Comparative example 2 (D2)
A trickle bed reactor A2' which differs from the trickle bed reactor A1 described in example 1 only in that:
the liquid redistributors 6 are not arranged in the reactor housing 10.
M-xylylenediamine B2 'was produced by the method of example 1 using the trickle bed reactor A2' described above.
The obtained m-xylylenediamine B2' was analyzed by the liquid chromatography external standard method, and the analysis results are shown in Table 1.
Comparative example 3 (D3)
M-xylylenediamine B3' was produced by the method of example 1 using the trickle bed reactor A1 described above; and differs from embodiment 1 only in that:
the pulse frequency of the three-dimensional pulse filler 5 is 15s -1 。
The obtained m-xylylenediamine B3' was analyzed by the liquid chromatography external standard method, and the analysis results are shown in Table 1.
In examples 1 to 8 and comparative examples 1 to 3, the liquid phase materials from the liquid outlet 9 were analyzed by liquid chromatography external standard method at the beginning of the catalyst operation in the catalytic hydrogenation reaction, 2000 hours and 3000 hours, respectively, and the analysis results are shown in table 1.
The results of the catalytic hydrogenation reactions at various time points are shown in Table 1
As can be seen from the comparison of examples 1 to 8 and comparative examples 1 to 3 and the data in Table 1, when m-xylylenediamine is produced by the method of the present invention using the trickle bed reactor of the present invention, the conversion rate of m-phthalonitrile and the molar yield of m-xylylenediamine are both high, and the relatively good yield can be maintained for a long period of time;
as is apparent from the comparison of example 1 and comparative example 1, the conversion rate of isophthalonitrile and the molar yield of m-xylylenediamine are significantly improved when the trickle-bed reactor is filled with the three-dimensional pulse filler 5;
as is apparent from a comparison of example 1 and comparative example 2, the trickle-bed reactor according to the present invention was used, and the three-dimensional pulse packing 5 in the trickle-bed reactor was used in combination with the liquid redistributor 6, and the conversion rate of isophthalonitrile and the molar yield of isophthalamide were both high when preparing isophthalamide according to the method of the present invention; if only the three-dimensional pulse packing 5 is arranged in the trickle bed reactor and no liquid redistributor 6 is matched with the trickle bed reactor, the conversion rate of isophthalonitrile and the molar yield of m-xylylenediamine are slightly reduced;
as is apparent from a comparison of example 1 and comparative example 3, when m-xylylenediamine is prepared using the trickle bed reactor according to the present invention and the method according to the present invention, the pulse frequency of the three-dimensional pulse packing 5 can affect the conversion rate of m-xylylenediamine and the molar yield of m-xylylenediamine, as well as the service life of the catalyst.
While the present invention has been described in detail through the foregoing description of the preferred embodiment, it should be understood that the foregoing description is not intended to limit the invention. Those skilled in the art will appreciate that many modifications and adaptations of the invention are possible and can be made with the teaching of the present specification. Such modifications and adaptations are intended to be within the scope of the present invention as defined in the appended claims.
Claims (10)
1. Trickle bed reactor, characterized in that it comprises a reactor shell (10);
a liquid distributor (2), at least one liquid redistributor (6) and at least one layer of supporting plate (7) are sequentially arranged in the reactor shell (10) from top to bottom at intervals, and the reactor shell is sequentially divided into a gas cavity, at least 2 catalyst beds (4) and a liquid cavity from top to bottom; the catalyst bed layer (4) is filled with a three-dimensional pulse filler (5);
the top of the reactor shell (10) is provided with a gas phase inlet (1), the bottom is provided with a liquid outlet (9), the side wall of the reactor shell is provided with a liquid inlet (3) corresponding to the liquid distributor (2), and the side wall of the reactor shell is provided with a gas outlet (8) corresponding to the liquid cavity;
the three-dimensional pulse packing (5) comprises three-dimensional pulse tube bundles vertically arranged in the catalyst bed layer (4), wherein each three-dimensional pulse tube bundle comprises a plurality of three-dimensional pulse tubes (51) which are arranged in parallel and in a dispersed mode, each three-dimensional pulse tube (51) is provided with a first vertical liquid channel, and a second vertical liquid channel is formed between every two adjacent three-dimensional pulse tubes (51).
2. The trickle bed reactor according to claim 1, wherein,
the three-dimensional pulse tube (51) comprises contraction sections (511) and expansion sections (512) which are alternately arranged along the length direction of the three-dimensional pulse tube, and the adjacent contraction sections (511) and expansion sections (512) form a pulse unit; the stereoscopic pulse tube (51) comprises 50-200 pulse units;
preferably, the area of the largest cross section in the pulse unit is 10-50mm 2 The method comprises the steps of carrying out a first treatment on the surface of the And/or
The area ratio of the smallest cross section to the largest cross section in the pulse unit is 0.01-0.25.
3. The trickle bed reactor according to claim 2, wherein,
the length ratio of the expansion section (512) to the contraction section (511) is 1/3-1; and/or
The ratio of the specific surface area of the expansion section (512) to the contraction section (511) is 1-3.
4. The trickle bed reactor according to claim 2 or 3, wherein,
the length of the contraction section (511) is 5-15mm; and/or
The specific surface area of the contraction section (511) is 1-5m 2 /m 3 。
5. The trickle bed reactor according to any one of claims 2-4, wherein,
in the three-dimensional pulse packing (5), the three-dimensional pulse tube bundles are arranged in the catalyst bed (4) in the following manner: adjacent 3 of the three-dimensional pulse tubes (51) are arranged in a regular triangle, forming a minimum arrangement unit.
6. The trickle bed reactor according to claim 5, wherein,
in the minimum arrangement unit, the arrangement directions of adjacent 2 stereoscopic pulse tubes (51) differ by 120 °; and/or
In the minimum arrangement unit, the distance between every two adjacent 2 stereoscopic pulse tubes (51) is L1 according to the distance between the vertical central axes of the two stereoscopic pulse tubes, and the length of the longest side of the maximum cross section in the pulse unit is L2, so that L1/L2=0.5-5.
7. A method of producing m-xylylenediamine using the trickle bed reactor of any one of claims 1-6, comprising:
(1) Introducing hydrogen gas from the gas phase inlet (1) into the trickle bed reactor to activate the catalyst filled in the catalyst bed (4);
(2) Introducing a composite solvent dissolved with isophthalonitrile into the trickle bed reactor from the liquid inlet (3), carrying out catalytic hydrogenation reaction on the catalyst bed (4) and the introduced hydrogen to prepare m-xylylenediamine, and outputting the m-xylylenediamine from the liquid outlet (9).
8. The method according to claim 7, wherein the pulse frequency of the stereoscopic pulse filler (5) in the trickle bed reactor is 0.01-10s -1 。
9. The method according to claim 7 or 8, wherein,
the catalyst filled in the catalyst bed layer (4) is a nickel catalyst;
preferably, the nickel-based catalyst is a framework-type catalyst or a supported catalyst, and the nickel content is more than or equal to 5wt%.
10. The method according to any one of claims 7 to 9, wherein,
the compound solvent comprises any two or more of tetrahydrofuran, methanol, toluene, cyclohexane, liquid ammonia and N-methyl pyrrolidone; and/or
In the catalytic hydrogenation reaction, the molar ratio of isophthalonitrile to hydrogen to composite solvent is 1 (1-10) (2-40); and/or
In the catalytic hydrogenation reaction, the reaction pressure is 6-20MPa, and/or the reaction temperature is 50-100 ℃.
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