CN114432988A - Continuous microwave reaction device and application thereof - Google Patents

Continuous microwave reaction device and application thereof Download PDF

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Publication number
CN114432988A
CN114432988A CN202011204191.5A CN202011204191A CN114432988A CN 114432988 A CN114432988 A CN 114432988A CN 202011204191 A CN202011204191 A CN 202011204191A CN 114432988 A CN114432988 A CN 114432988A
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microwave
reaction
continuous
reaction tube
radiator
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杨柳
李腾飞
任靖
武永安
石勤智
周岩
赵保槐
李柯志
胡海强
苏海霞
韩帅
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China Petroleum and Chemical Corp
Sinopec Catalyst Co
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China Petroleum and Chemical Corp
Sinopec Catalyst Co
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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
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J19/12—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electromagnetic waves
    • B01J19/122—Incoherent waves
    • B01J19/126—Microwaves
    • 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
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/08—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y
    • B01J29/085—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y containing rare earth elements, titanium, zirconium, hafnium, zinc, cadmium, mercury, gallium, indium, thallium, tin or lead
    • B01J29/088—Y-type faujasite
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/30—Ion-exchange
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/34—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation
    • B01J37/341—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation
    • B01J37/344—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of electromagnetic wave energy
    • B01J37/346—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of electromagnetic wave energy of microwave energy
    • 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
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00002—Chemical plants
    • B01J2219/00027—Process aspects
    • B01J2219/00033—Continuous 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
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/12—Processes employing electromagnetic waves
    • B01J2219/1203—Incoherent waves
    • B01J2219/1206—Microwaves
    • B01J2219/1209—Features relating to the reactor or vessel
    • B01J2219/1221—Features relating to the reactor or vessel the reactor per se
    • 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
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/12—Processes employing electromagnetic waves
    • B01J2219/1203—Incoherent waves
    • B01J2219/1206—Microwaves
    • B01J2219/1248—Features relating to the microwave cavity
    • B01J2219/1266—Microwave deflecting parts
    • 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
    • B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
    • B01J2229/10—After treatment, characterised by the effect to be obtained
    • B01J2229/18—After treatment, characterised by the effect to be obtained to introduce other elements into or onto the molecular sieve itself
    • B01J2229/186—After treatment, characterised by the effect to be obtained to introduce other elements into or onto the molecular sieve itself not in framework positions

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Abstract

The invention relates to the technical field of catalyst preparation, and discloses a continuous microwave reaction device and application thereof. This continuous microwave reaction unit includes microwave generator (1), microwave converter (2), microwave radiator (3), microwave reaction chamber (4) and reaction tube (5), microwave generator (1) microwave converter (2) with microwave radiator (3) connect gradually, and microwave generator (1), microwave converter (2) set up the outside of microwave reaction chamber (4), microwave radiator (3) set up the inside in microwave reaction chamber (4), reaction tube (5) winding microwave radiator (3) set up. The continuous microwave reaction device provided by the invention has the advantages of uniform microwave radiation and high heating efficiency, and can realize continuous production.

Description

Continuous microwave reaction device and application thereof
Technical Field
The invention relates to the technical field of catalyst preparation, in particular to a continuous microwave reaction device and application thereof.
Background
With the continuous progress of molecular sieve synthesis method and modification means, the scale of molecular sieve industrial production is gradually enlarged. At present, a hydrothermal method is generally adopted for industrially preparing the molecular sieve, and the cation of the molecular sieve prepared by the hydrothermal method is sodium ion in general, but in practical application, the sodium ion in the molecular sieve needs to be exchanged into other cations such as hydrogen ion, potassium ion, rare earth metal ion and the like according to specific conditions, so that the molecular sieve has a specific catalytic function.
Ion exchange of molecular sieves is usually carried out in aqueous solution, and the exchange is generally carried out industrially on a vacuum belt filter or in an exchange tank in a batch tank-exchange manner. With the increasingly strict requirements of national and local governments on the wastewater discharged by enterprises, the treatment cost of the waste liquid generated by the molecular sieve ion exchange process is increased year by year, and the enterprises face huge environmental protection pressure and economic pressure. In order to improve the ion exchange degree and reduce the content of residual sodium in the molecular sieve, the method is generally realized by alternately carrying out multiple exchange and high-temperature roasting, namely, the production is carried out by adopting a process of 'two-way exchange and one-way roasting' or 'two-way exchange and two-way roasting'.
Because the exchange cations exist in the form of hydrated ions in an aqueous solution, and the radius of the hydrated ions is large, the exchange cations cannot enter small pore channels of the molecular sieve in the ion exchange process, for example, the exchange cations are difficult to enter sodalite cages (also called beta cages) and hexagonal column cages of the Y-type molecular sieve to complete exchange, Na + in the beta cages needs to be migrated out and then exchanged through high-temperature roasting, but the high-temperature roasting affects the crystal structure of the molecular sieve. Therefore, the production process of exchanging and modifying the molecular sieve by using the traditional preparation process has the problems of low ion exchange efficiency, long exchange time, long production process flow, high production cost and the like. In order to achieve the exchange degree required by industry through only one exchange of exchange ions, researchers have tried to adopt a hot-pressing exchange method, but the long-time high-temperature and high-pressure exchange condition not only increases the energy consumption of production, but also destroys the crystal structure of the molecular sieve to different degrees. Therefore, the development of efficient ion exchange process has become a research hotspot in the molecular sieve industry today.
The chemical reaction usually needs heating or high temperature and high pressure, the traditional heating method uses heat conduction and heat convection, but the reaction speed is relatively slow, the reaction yield and selectivity are not high, and with the development of the current science and technology, the important problems to be solved by people are that the chemical reaction speed is accelerated, the reaction yield is increased, the post-treatment process is simplified, the reaction selectivity is improved, and the production efficiency is improved. And because of the current requirement of environmental protection, the conventional reaction kettle needs fewer and fewer steam boilers, and the application of the steam heating reaction kettle is greatly limited.
In 1986, the first article of microwave-catalyzed chemical synthesis was published by the university of geodie, canada, who uses a microwave electromagnetic field as a means for accelerating chemical reactions in a domestic microwave oven, and found that microwaves can significantly increase the esterification reaction rate of benzoic acid and alcohol and increase the yield. Since then, microwave assisted chemistry has attracted a great deal of attention. Microwave as a new energy has the advantages of internal heating, rapid heating, selective heating, energy conservation, environmental protection and the like, can greatly improve the chemical reaction speed, has higher efficiency (the highest efficiency can be improved by 1240 times) by dozens of times or even hundreds of times than that of a conventional heating method, and has been widely applied to a plurality of fields of chemical engineering, materials, petroleum, metallurgy and the like.
At present, scientific research and production have higher practicability requirements on microwave chemical reaction devices, how to enable the efficient, energy-saving and environment-friendly microwave chemical reaction devices to meet different production requirements of various industries, and provide new challenges for the traditional microwave chemical reaction devices in the aspects of reaction pressure, working power, temperature control and the like. For example, CN108355595A discloses a continuous pipeline reactor capable of continuous production, which is designed by utilizing the special catalytic action of microwave on chemical reactants, and utilizes microwave to strengthen chemical reaction conditions, thereby greatly shortening chemical reaction time, realizing continuous and safe operation of chemical materials in a completely closed fine space, and simultaneously preventing waste materials in the reaction process from exposing air to pollute the environment. The invention has the advantages of improving the reaction speed, saving energy and reducing consumption; the reaction is safe, the materials are subjected to chemical or physical reaction in the pipeline, and the residence amount is small; even if overheating and explosion occur, the environment cannot be affected safely; the method is environment-friendly, the reaction is carried out in a completely closed environment, no gas or liquid is leaked, and no environmental pollution is caused. But the microwave catalytic continuous pipeline reactor designed by the invention is difficult to bear chemical reaction with higher temperature and pressure; a similar tube flow microwave reactor design is disclosed in CN 208066340U; CN110605080A discloses a high-pressure microchannel leading-in type microwave reactor, which adopts a microchannel leading-in mode, and by reducing the pressure bearing area of a hole, the pressure bearing capacity in a kettle is enhanced, the catalysis promotion effect of microwaves is fully embodied, and meanwhile, microwaves are led into a cavity of the reaction kettle from a microchannel at the bottom of the reaction kettle by a metal belt by utilizing an antenna effect, so that the microwaves are more uniform in the cavity of the reaction kettle, the microwave heating cold spots are reduced, and the energy utilization efficiency is improved. However, in the design, the depth of the micro-channel introduced into the reaction kettle is shallow, so that the penetration depth of the microwave is limited, and the micro-channel is introduced from the bottom, so that the effect of uniform microwave radiation in the whole reaction kettle cannot be achieved; CN104667849A discloses a high-power microwave reactor and a microwave continuous pressure reaction system. Including microwave generator, waveguide, serpentine waveguide, reaction cavity and reaction tube, the microwave that microwave generator produced passes through the waveguide and conducts again to serpentine waveguide, serpentine waveguide follows reaction cavity's surface laminating extends the setting, serpentine waveguide with reaction cavity surface contact department is provided with microwave transmission window, the reaction tube runs through reaction cavity. The serpentine waveguide extends on the surface of the reaction cavity, so that the microwave can be absorbed by the microwave transmission window on a large area of more than one surface of the reaction cavity. Although the design increases the area of the reaction cavity body irradiated by the microwave, the limitations of microwave energy attenuation and limited microwave penetration depth can not be avoided; CN110064353A discloses a spiral coil pipe formula microwave reactor, including microwave excitation chamber, compression excitation chamber, locating rack, spiral coil pipe, microwave source, be equipped with the compression excitation chamber in the microwave excitation chamber, be equipped with the locating rack between microwave excitation chamber and the compression excitation chamber, the spiral coil pipe is installed to the locating rack, spiral coil pipe both ends are equipped with solution inlet and solution outlet respectively, and, solution inlet and solution outlet are located the microwave excitation chamber outer wall, the microwave excitation chamber outer wall is equipped with a plurality of microwave sources. The structural design can improve the electric field intensity and uniformity, increase the irradiation time and improve the reaction efficiency. Thus, the above-mentioned prior art microwave reactor technology exists: 1. in the conventional waveguide type microwave reaction kettle, because the penetration depth of microwaves in a reaction medium system is shallow, the phenomenon of nonuniform microwave radiation is difficult to avoid. The microwave radiation energy close to the microwave source end is large, a microwave gathering point is generated, the local overheating phenomenon of a reaction system is caused, the microwave radiation quantity far away from the source end is small, the problem of non-uniformity of the temperature and the reactant state in the reaction system is caused, and the controllability of the reaction process is poor; 2. the conventional microwave tubular reactor is limited by the selection of materials of equipment, and often cannot bear certain working pressure, particularly cannot bear a long-time high-temperature and high-pressure working environment; 3. the reaction materials have short retention time in the microwave tubular reactor and cannot fully react; 4. the existing microwave reactor has small reaction scale, and a lot of work is only carried out on laboratory scale, so that accurate data and the like cannot be provided for realizing large-scale chemical reaction application and designing microwave pilot-scale reactor equipment. Therefore, it also hinders the application of large-scale, continuous industrial production.
Disclosure of Invention
The invention aims to solve the problems of insufficient microwave penetration depth, nonuniform irradiation and the like in a microwave reactor in the prior art, and provides a continuous microwave reaction device and application thereof.
In order to achieve the above object, a first aspect of the present invention provides a continuous microwave reaction apparatus, including a microwave generator, a microwave converter, a microwave radiator, a microwave reaction chamber, and a reaction tube, wherein the microwave generator, the microwave converter, and the microwave radiator are connected in sequence, and the microwave generator and the microwave converter are disposed outside the microwave reaction chamber, the microwave radiator is disposed inside the microwave reaction chamber, and the reaction tube is disposed around the microwave radiator.
Preferably, the microwave reaction cavity is provided with a gas inlet and a gas outlet.
Preferably, the reaction device comprises a pressure measuring unit which is arranged inside the microwave reaction cavity and used for measuring the pressure in the microwave reaction cavity.
Preferably, the reaction tube has a U-shape, a V-shape, a W-shape, a spiral shape, or a double spiral shape.
Preferably, one end of the reaction tube is connected with the feed inlet, and the other end of the reaction tube is connected with the discharge outlet.
Preferably, the reaction tube is a wave-transparent material.
Preferably, the diameter of the reaction tube is 2-200 mm, and the working pressure is 0-4 MPa.
Preferably, the flow rate of the materials in the reaction tube is 0.1-100L/min.
Preferably, a sealing assembly is arranged at the connecting position of the microwave radiator and the microwave reaction cavity.
Preferably, the frequency of the microwave magnetron in the microwave generator is 2430-.
Preferably, the number of the microwave magnetrons is one or more.
Preferably, the output power of the microwave generator is 0.001-50 KW.
Preferably, the reaction device further comprises a temperature measuring unit arranged on the reaction tube and used for measuring the temperature of the materials in the reaction tube.
Preferably, the reaction device further comprises a water loading unit for protecting the microwave generator from overload.
In a second aspect, the invention provides the use of a continuous microwave reactor according to the invention for the preparation of a catalyst, preferably for a molecular sieve ion exchange reaction.
By the technical scheme, the flow path of the continuous flow reaction materials is increased, the residence time under the action of microwave radiation is prolonged, the continuous flow reaction materials can absorb microwaves in the whole microwave reaction cavity, the uniformity of microwave radiation is improved, and continuous production can be realized.
Drawings
FIG. 1 is a schematic structural view of a continuous microwave reaction apparatus according to the present invention.
Description of the reference numerals
1. Microwave generator 2, microwave converter
3. Microwave radiator 4 and microwave reaction cavity
41. Gas inlet 42, gas outlet
5. Reaction tube 51, feed inlet
52. Discharge port 6 and sealing assembly
7. Temperature measuring unit 8 and pressure measuring unit
Detailed Description
The following detailed description of embodiments of the invention refers to the accompanying drawings. It should be understood that the detailed description and specific examples, while indicating the present invention, are given by way of illustration and explanation only, not limitation.
The endpoints of the ranges and any values disclosed herein are not limited to the precise range or value, and such ranges or values should be understood to encompass values close to those ranges or values. For ranges of values, between the endpoints of each of the ranges and the individual points, and between the individual points may be combined with each other to give one or more new ranges of values, and these ranges of values should be considered as specifically disclosed herein.
The continuous microwave reactor apparatus of the present invention is described in further detail below with reference to the attached drawing figures, wherein like numerals indicate like features throughout.
The invention provides a continuous microwave reaction device which comprises a microwave generator 1, a microwave converter 2, a microwave radiator 3, a microwave reaction cavity 4 and a reaction tube 5, wherein the microwave generator 1, the microwave converter 2 and the microwave radiator 3 are sequentially connected, the microwave generator 1 and the microwave converter 2 are arranged outside the microwave reaction cavity 4, the microwave radiator 3 is arranged inside the microwave reaction cavity 4, and the reaction tube 5 is wound around the microwave radiator 3.
According to the continuous microwave reaction device provided by the invention, the reaction tube is wound around the periphery of the microwave radiator, so that a continuous flow reaction material flow path is increased, the retention time under the action of microwave radiation is prolonged, the microwave radiator is positioned in the middle of the spiral continuous reaction tube and penetrates through the spiral reaction tube, the continuous flow reaction material can absorb microwaves in the whole reaction cavity, the uniformity of microwave radiation is improved, and the problems of insufficient depth and non-uniformity of microwave penetration of a common microwave reactor are effectively avoided.
The microwave radiator with the gap is a coaxial gap radiator, and the microwave radiator adopts a coaxial gap structure to radiate energy to the surrounding space, namely the coaxial gap radiator. While the general radiation radiator generates electromagnetic waves directly from the current element on the conductor plane, the microwave radiator (coaxial slot radiator) in this application radiates outward through the slot between the conductor plane and the conductor plane, as compared with the general radiation radiator, and the radiation can be regarded as being generated by the equivalent field source-magnetic current element on the slot, and the electromagnetic waves are radiated outward through the slot by cutting a plurality of openings (slots) on the same axis. For example, specifically: a plurality of uniformly distributed inclined slits are arranged on the coaxial line outer conductor at preset intervals, and omnidirectional radiation can be obtained in a horizontal plane. Therefore, the microwave radiator in the application can realize the uniformity and the omnidirectionality of the microwave radiation through the opening direction, the number and the distribution of the gaps according to the requirements.
FIG. 1 is a schematic structural view of a continuous microwave reaction apparatus according to the present invention. As shown in fig. 1, the continuous microwave reaction device comprises a microwave generator 1, a microwave converter 2 and a microwave radiator 3 which are connected in sequence, wherein the microwave generator 1 and the microwave converter 2 are arranged outside a microwave reaction cavity 4, the microwave radiator 3 is arranged inside the microwave reaction cavity 4, and a reaction tube 5 is wound around the microwave radiator 3.
In order to meet the requirements of the reaction medium system on different pressures and monitor the reaction pressure in the cavity, in the invention, a gas inlet 41 and a gas outlet 42 are arranged on the microwave reaction cavity 4. The pressure in the cavity is adjusted through the air inlet and the air outlet, and the microwave irradiation high-pressure reaction under certain balance pressure can be maintained.
The shell of the microwave reaction cavity is made of metal to form a closed space, so that the pressure balance in the reaction cavity can be maintained, and the pressure balance in the cavity can also be maintained by adjusting the air inlet and the air outlet which are arranged on the shell.
In order to further satisfy the requirements of the reaction medium system for different pressures, in the present invention, it is preferable that the reaction device includes a pressure measuring unit 8 disposed inside the microwave reaction chamber 4 for measuring the pressure inside the microwave reaction chamber 4. As shown in fig. 1, a gas inlet 41 and a gas outlet 42 are disposed on the microwave reaction chamber 4, and the gas inlet and the gas outlet are used to maintain pressure balance in the chamber, so that the pressure inside and outside the continuous flow reaction tube therein is balanced, thereby avoiding the problem that a common microwave tube reactor cannot withstand a high-temperature and high-pressure working environment.
In order to sufficiently act on the material flowing through the reaction tube, in the present invention, it is preferable that the reaction tube 5 has a U-shape, a V-shape, a W-shape, a spiral shape or a double spiral shape. Through setting to different shapes, increased continuous flow reaction material and flowed through the route, prolonged simultaneously and received microwave radiation effect dwell time, and microwave radiator is fixed in the continuous reaction tube middle part and passes the reaction tube for continuous flow reaction material all can absorb the microwave in whole reaction cavity within range, has further promoted microwave radiation's homogeneity.
In order to further ensure the normal and stable operation of the microwave radiator, in the present invention, it is preferable that the reaction tube 5 is made of wave-transparent material. By adopting the wave-transparent material, the penetration of the microwave in the reaction medium system is not affected, and the phenomenon of nonuniform microwave radiation is avoided.
The wave-transmitting material may include, for example, a polymer material, a composite engineering material, a glass material, a ceramic material, a composite of the above materials, or the like.
In order to meet the requirements of a reaction medium system on different pressures, in the invention, the diameter of the reaction tube 5 is preferably 2-200 mm, and the working pressure is preferably 0-4 MPa; more preferably, the diameter of the reaction tube 5 is 3-100 mm, and the working pressure is 0.1-2.5 MPa. As shown in fig. 1, one end of the reaction tube 5 is connected to the inlet 51, the other end is connected to the outlet 52, and the inlet and outlet are outside the microwave reaction cavity.
In order to fully act on the materials flowing through the reaction tube, in the invention, the flow speed of the materials in the reaction tube 5 is preferably 0.1-100L/min; more preferably, the flow rate of the material in the reaction tube 5 is 1 to 20L/min. The phenomenon that the materials flowing through are unevenly radiated by microwaves is further ensured by controlling the diameter and the working pressure of the reaction tube and the flow rate of the materials in the reaction tube.
In the present invention, it is preferable that a sealing assembly 6 is provided at a connecting position of the microwave radiator 3 and the microwave reaction chamber 4. The sealing assembly can prevent microwave leakage and can bear the working pressure within the range of 0-10 MPa. As shown in fig. 1, the microwaves generated by the microwave generator 1 are transmitted to the microwave radiator 3 through the sealing assembly 6 and then through the microwave converter 2.
In order to meet the requirements of the reaction medium system to be treated, in the present invention, preferably, the frequency of the microwave magnetron in the microwave generator 1 is 2430-; more preferably 2440 and 2460MHz, and in one embodiment of the invention, a 2450MHz microwave magnetron is used.
In order to further satisfy the requirement of the reaction medium system to be treated, in the present invention, it is preferable that the number of the microwave magnetrons is one or more.
In order to further meet the requirement of a reaction medium system to be treated, in the invention, the output power of the microwave generator 1 is preferably 0.001-50 KW; more preferably, the output power of the microwave generator 3 is 0.01-40 KW. The output microwave power output can be adjusted manually or automatically by a reaction condition controller.
In order to monitor the reaction temperature in the reaction tube, in the present invention, it is preferable that the continuous microwave reaction apparatus further comprises a temperature measuring unit 7 disposed on the reaction tube 5 for measuring the temperature of the material in the reaction tube 5. As shown in fig. 1, the reaction tube 5 is provided with a temperature measuring unit 7, and the temperature inside the reaction tube 5 is monitored by the temperature measuring unit.
In order to further ensure long-term, safe operation of the microwave reactor, in the present invention, it is preferable that the reaction apparatus further comprises a water loading unit provided on the microwave generator 1 for including protection of the microwave generator 1 from overload. By arranging the water load unit, the microwave generator is prevented from being burnt out when no reaction material is introduced into the continuous flow reaction tube.
In a second aspect, the present invention provides the use of a continuous microwave reactor according to the present invention for the preparation of a catalyst, preferably for ion exchange reactions.
The specific method for utilizing the continuous microwave reaction device in the molecular sieve ion exchange reaction comprises the following steps:
the reaction material containing the sodium type molecular sieve and the solution to be exchanged flows into the reaction tube from the feed inlet of the reaction tube and enters the cavity of the microwave reactor; under the action of microwave radiation of a microwave radiator, a sodium molecular sieve in a continuous flow reaction coil is contacted with a solution to be exchanged to carry out ion exchange reaction, a continuous flow reaction material system is heated under the action of microwave radiation and carries out ion exchange, the continuous flow reaction material after the ion exchange flows out of a cavity of a microwave reactor from an outlet of the reaction tube, and the molecular sieve after the ion exchange is subjected to solid-liquid filtration separation and water washing to obtain the molecular sieve after the exchange.
Wherein, the sodium type molecular sieve can be one or more of a molecular sieve commonly used in catalyst preparation, a Y type molecular sieve, an X type molecular sieve, an A type molecular sieve, a ZSM-5 molecular sieve and a beta type molecular sieve; after the reaction materials are added into the reaction kettle, the pre-charging pressure can be 0-2.5 MPa, and the pressure balance is maintained through the air inlet and the air outlet along with the reaction. The continuous flow reaction material is radiated by a microwave radiator in a reaction tube under the action of microwave, the output power of the microwave reactor device can be adjusted according to the feeding liquid amount (or flow rate) except for the specified microwave heating frequency, the exchange temperature is from the initial inlet temperature to 250 ℃, the heating time of the heating section is 10 s-40 min, the preferred exchange temperature is 70-220 ℃, and the constant temperature exchange time is 30 s-1 h. And (3) allowing the continuous flow reaction material to flow out from the outlet of the reaction tube after microwave-assisted ion exchange, performing solid-liquid separation by adopting conventional filtering equipment, and washing by adopting deionized water to obtain the exchanged molecular sieve.
Example 1
The microwave reactor device shown in fig. 1 is adopted, and comprises a microwave generator 1, a microwave converter 2 and a microwave radiator 3 (specifically, a coaxial slot radiator) which are connected in sequence, wherein the microwave generator 1 and the microwave converter 2 are arranged outside a microwave reaction cavity 4, the microwave radiator 3 is arranged inside the microwave reaction cavity 4, and a spiral reaction tube 5 is wound on the microwave radiator 3. The microwave reaction cavity 4 is provided with a gas inlet 41 and a gas outlet 42, the microwave reaction cavity 4 is internally provided with a pressure measuring unit 8, one end of the reaction tube 5 is connected with the feed inlet 51, the other end of the reaction tube is connected with the discharge outlet 52, the material inlet and the material outlet are both arranged outside the microwave reaction cavity, and the reaction tube 5 is provided with a temperature measuring unit 7.
Specifically, the NaY type molecular sieve is contacted with an aqueous solution containing rare earth chloride to form a reaction system to be exchanged, the weight ratio of water to NaY in the reaction system to be exchanged is 10:1, and the weight ratio of rare earth to NaY is 0.5: 1. The exchange reaction system flows into a pressure-balanced microwave reaction cavity 4 from a reaction tube feeding hole 51, and the balanced working pressure in the reaction cavity is 2 MPa. The continuous flow reaction material is heated by microwave with the frequency of 2450MHz and the output power of 6KW, and the molecular sieve ion exchange reaction is carried out under the microwave irradiation. The flow rate of the materials in the reaction tube is 0.2L/min, the time of the continuous flow materials flowing through the heating section is 15min, the materials are heated to 180 ℃ from 25 ℃ of the inlet end by microwave, then flow through the constant temperature exchange section, the materials are exchanged for 10min at the constant temperature of 180 ℃ under the microwave irradiation and then flow out from the outlet of the reaction tube, and the materials after the ion exchange reaction are filtered and washed to obtain the exchanged molecular sieve with the residual sodium oxide content of 1.2%.
The continuous microwave reaction device is fixed in the microwave reaction cavity through the continuous reaction tube, penetrates through the reaction cavity and is spirally wound on the periphery of the microwave radiator, so that a continuous flow reaction material flow path is increased, the retention time under the action of microwave radiation is prolonged, the microwave radiator is fixed in the middle of the spiral continuous reaction tube and penetrates through the spiral reaction tube, the continuous flow reaction material can absorb microwaves in the whole reaction cavity, the uniformity of microwave radiation is improved, and the controllability of a reaction process is enhanced. Meanwhile, a certain balance pressure is maintained in the microwave reaction cavity, so that the internal and external pressure difference of the reaction tube is reduced or even eliminated, the difficulty in selecting the type of the reaction tube is greatly reduced, the microwave reactor body is effectively protected, and the continuous microwave reaction under the high-temperature and high-pressure environment can be realized. By applying the microwave continuous reactor to the molecular sieve ion exchange reaction, compared with the conventional molecular sieve ion exchange process, the problems of non-uniformity and low heating efficiency of conventional conduction heating are solved, and the molecular sieve ion exchange balance can be quickly reached so that the catalytic active center of the modified molecular sieve can achieve controllability.
The preferred embodiments of the present invention have been described in detail above with reference to the accompanying drawings, but the present invention is not limited thereto. Within the scope of the technical idea of the invention, numerous simple modifications can be made to the technical solution of the invention, including combinations of the individual specific technical features in any suitable way. The invention is not described in detail in order to avoid unnecessary repetition. Such simple modifications and combinations should be considered within the scope of the present disclosure as well.

Claims (10)

1. The utility model provides a continuous microwave reaction unit, includes microwave generator (1), microwave converter (2), microwave radiator (3), microwave reaction chamber (4) and reaction tube (5), its characterized in that, microwave generator (1) microwave converter (2) with microwave radiator (3) connect gradually, and microwave generator (1), microwave converter (2) set up the outside in microwave reaction chamber (4), microwave radiator (3) set up the inside in microwave reaction chamber (4), reaction tube (5) winding microwave radiator (3) set up.
2. The continuous microwave reactor according to claim 1, wherein the microwave reaction chamber (4) is provided with a gas inlet (41) and a gas outlet (42);
preferably, the reaction device comprises a pressure measuring unit (8) which is arranged inside the microwave reaction cavity (4) and is used for measuring the pressure in the microwave reaction cavity (4).
3. The continuous microwave reaction device according to claim 1, wherein the reaction tube (5) has a shape of U-shape, V-shape, W-shape, spiral shape or double spiral shape;
preferably, one end of the reaction tube (5) is connected with the feed inlet (51), and the other end is connected with the discharge outlet (52).
4. The continuous microwave reaction device according to claim 1, wherein the reaction tube (5) is of wave-transparent material.
5. The continuous microwave reactor according to claim 1, wherein the diameter of the reaction tube (5) is 2 to 200mm, and the working pressure is 0 to 4 MPa;
preferably, the flow rate of the materials in the reaction tube (5) is 0.1-100L/min.
6. Continuous microwave reaction unit according to claim 1, wherein a sealing assembly (6) is provided at the connection point of the microwave radiator (3) and the microwave reaction chamber (4).
7. The continuous microwave reaction apparatus according to claim 1, wherein the frequency of the microwave magnetron in the microwave generator (1) is 2430-2470 MHz;
preferably, the number of the microwave magnetrons is one or more;
preferably, the output power of the microwave generator (1) is 0.001-50 KW.
8. The continuous microwave reactor according to claim 1, wherein the reactor further comprises a temperature measuring unit (7) disposed on the reaction tube (5) for measuring the temperature of the material in the reaction tube (5).
9. The continuous microwave reaction device according to claim 1, wherein the reaction device further comprises a water loading unit provided on the microwave generator (1) for including protecting the microwave generator (1) from overload.
10. Use of a continuous microwave reaction unit according to any one of claims 1 to 9 for the preparation of a catalyst, preferably for a molecular sieve ion exchange reaction.
CN202011204191.5A 2020-11-02 2020-11-02 Continuous microwave reaction device and application thereof Pending CN114432988A (en)

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Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102458644A (en) * 2009-04-15 2012-05-16 C-技术创新有限公司 Electromagnetic heating reactor and improvements
CN103623755A (en) * 2013-11-18 2014-03-12 陕西科技大学 Industrial continuous type microwave reactor
CN104383866A (en) * 2014-12-08 2015-03-04 华东理工大学 Microwave reaction device using coaxial leaky antenna and application of microwave reaction device using coaxial leaky antenna
CN104667849A (en) * 2015-02-06 2015-06-03 南京博炫生物科技有限公司 High-power microwave reactor and microwave continuous pressure reaction system
CN106334508A (en) * 2016-08-31 2017-01-18 电子科技大学 Continuous transmission type focusing microwave reactor
US20180093247A1 (en) * 2015-03-20 2018-04-05 Cnr - Consiglio Nazionale Delle Ricerche Structure of integrated photochemical reactor
CN110064353A (en) * 2019-06-17 2019-07-30 深圳市弘玮环境技术有限公司 Coil microwave reactor

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102458644A (en) * 2009-04-15 2012-05-16 C-技术创新有限公司 Electromagnetic heating reactor and improvements
CN103623755A (en) * 2013-11-18 2014-03-12 陕西科技大学 Industrial continuous type microwave reactor
CN104383866A (en) * 2014-12-08 2015-03-04 华东理工大学 Microwave reaction device using coaxial leaky antenna and application of microwave reaction device using coaxial leaky antenna
CN104667849A (en) * 2015-02-06 2015-06-03 南京博炫生物科技有限公司 High-power microwave reactor and microwave continuous pressure reaction system
US20180093247A1 (en) * 2015-03-20 2018-04-05 Cnr - Consiglio Nazionale Delle Ricerche Structure of integrated photochemical reactor
CN106334508A (en) * 2016-08-31 2017-01-18 电子科技大学 Continuous transmission type focusing microwave reactor
CN110064353A (en) * 2019-06-17 2019-07-30 深圳市弘玮环境技术有限公司 Coil microwave reactor

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