CN111841469A - Tubular continuous flow ultrasonic reactor - Google Patents

Tubular continuous flow ultrasonic reactor Download PDF

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Publication number
CN111841469A
CN111841469A CN202010516802.3A CN202010516802A CN111841469A CN 111841469 A CN111841469 A CN 111841469A CN 202010516802 A CN202010516802 A CN 202010516802A CN 111841469 A CN111841469 A CN 111841469A
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tool head
ultrasonic
fluid
tubular continuous
wall
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董建
范晓梅
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/08Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J19/10Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing sonic or ultrasonic vibrations

Abstract

The invention relates to the technical field of ultrasonic equipment, and discloses a tubular continuous flow ultrasonic reactor which comprises an ultrasonic transducer, an amplitude transformer, a tool head and a fluid pipeline, wherein one end of the amplitude transformer is connected with the ultrasonic transducer, the other end of the amplitude transformer is connected with the tool head, the fluid pipeline is wound and arranged on a vibration wall of the tool head, ultrasonic waves are reflected at the vibration wall to generate radial resonance standing waves, and the vibration wall of the tool head is positioned at an antinode of the resonance standing waves. The sound wave is totally reflected at the vibration wall of the tool head, the reflected wave is superposed with the excitation wave to form a resonance standing wave along the radial direction of the tool head, the vibration wall is arranged at an antinode, and the energy of the ultrasonic wave is radiated from the vibration wall and is conducted into the fluid pipeline; the surface area of the vibrating wall is large, so that more fluid pipelines can be contacted, the volume of the fluid pipeline can be larger, and the ultrasonic reactor with large volume can be conveniently manufactured; in addition, the ultrasonic transducer is separated from the fluid pipeline through the amplitude transformer, so that the temperature rise caused by heat entering the fluid pipeline can be reduced.

Description

Tubular continuous flow ultrasonic reactor
Technical Field
The invention relates to the technical field of ultrasonic equipment, in particular to a tubular continuous flow ultrasonic reactor.
Background
The continuous reactor based on the micro-pipeline is widely applied to the field of synthesis of fine chemicals and medical materials due to the advantages of high heat and mass transfer speed, multi-phase popularity and controllability, safe process, low equipment cost, simplicity in operation, rapid amplification and the like, but the tubular reactors also have the problems of weak convection mixing, easiness in solid blockage and the like.
In general, the convection mixing can be enhanced by filling some fillers in the pipeline (such as static mixing internals) or designing the pipeline into a bent or deformed structure, but the passive mixing enhancement method has several disadvantages, firstly, the pressure drop of the flow system is increased by the mixing structure, and the large pressure drop is not beneficial to enlarging the volume of the reactor by increasing the length of the pipeline; secondly, the mixing method extremely depends on the flow velocity of the fluid, and has a good mixing effect only when the flow velocity is large, so that the mixing method has poor operation elasticity, a narrow operation window and is not beneficial to a process with long retention time; finally, the complex channel structure or packing further increases the risk of channel blockage by solids, especially for reactors with relatively small channel diameters, such as microreactors.
The active mixer strengthens the fluid mixing in the pipeline through an external field, can use an empty pipeline or a very simple pipeline structure (such as a straight pipeline), has small pressure drop, and can well solve the problems of weak convection mixing, easy blockage by solids and the like. In addition, the mixing effect of the method is mainly determined by the strength of an external field and does not depend on the flow velocity of the fluid, so that the mixing effect and the retention time can be separately adjusted, the operation interval is large, the elasticity is good, and the method is suitable for low-flow-velocity or high-flow-velocity operation; meanwhile, the method can prevent or dredge solid blockage in the pipeline by utilizing an external field.
Among these active mixers, ultrasound-based reactors are the most promising, since ultrasound is a mechanical wave, safe and reliable; meanwhile, equipment such as an ultrasonic cleaning machine and the like is large-scale and practical in the industry, and the equipment for generating the ultrasonic waves is mature in technology and low in cost. While ultrasound has been widely reported to enhance the mixing of fluids in pipelines, the design of ultrasonic tubular reactors is complicated by the need to combine the knowledge of two different disciplines of ultrasonic transducers and chemical reactors.
Several ultrasonic reactors have been reported, and world patent WO2011023761 discloses a method for introducing ultrasound into a pipeline reactor by directly transmitting ultrasound from an ultrasonic transducer to a process fluid in contact therewith through a coupling device and introducing ultrasonic energy into the reactor through the process fluid, which is mainly suitable for introducing ultrasound at reactor parts such as an inlet and an outlet because ultrasound is attenuated in the process fluid relatively fast. German patent DE10243837a1 discloses a high throughput ultrasonic flow cell reactor in which an ultrasonic probe is connected to a reactor tube via a jacket, and high pressure water is injected between the jacket and the reactor tube, the water not only being used to conduct ultrasonic waves into the pipe, but also being able to control the temperature of the pipe.
The Chinese patent with the publication number of CN104923468B and publication date of 2018.10.23 discloses a high-power ultrasonic micro-reactor, which is directly and rigidly connected with an ultrasonic transducer through a front radiation surface of the ultrasonic transducer, so that the micro-reactor and the ultrasonic transducer vibrate as a whole, and the wavelength of ultrasonic waves formed by vibration in a direction vertical to the front radiation surface is twice of the distance from the upper surface of the micro-reactor to the back surface of a back cover plate; the upper surface of the micro-reactor is the surface of one side of the micro-reactor far away from the ultrasonic transducer, the back surface of the back cover plate is the surface of one side of the back cover plate far away from the piezoelectric ceramic stack, and the distance from the upper surface of the micro-reactor to the back surface of the back cover plate is the length of the ultrasonic micro-reactor in the direction vertical to the front radiation surface.
The pipe body flow channel of the ultrasonic microreactor is positioned in a reactor plate, the reactor plate is combined with the front radiation surface of the sandwich transducer, and the whole device forms a half-wave oscillator in the longitudinal direction to achieve resonance so that ultrasonic energy is converged in a pipeline in the reactor plate. The reactor has high ultrasonic energy efficiency and simple structure, but ultrasonic amplification is difficult, the radiation area of the ultrasonic transducer is limited, the length of a pipeline which can be contacted is limited, and the reactor is not beneficial to being made into an ultrasonic reactor with large volume.
Disclosure of Invention
The purpose of the invention is: the utility model provides a tubular continuous flow ultrasonic reactor to solve the problem that the ultrasonic reactor ultrasonic transducer in the prior art has limited radiation area and limited length of the pipeline which can be contacted, and is not beneficial to being made into a large-volume ultrasonic reactor.
In order to achieve the above object, the present invention provides a tubular continuous flow ultrasonic reactor, which comprises an ultrasonic transducer, an amplitude transformer, a tool head and a fluid pipeline, wherein one end of the amplitude transformer is connected with the ultrasonic transducer, the other end of the amplitude transformer is connected with the tool head, the fluid pipeline is wound and arranged on a vibration wall of the tool head, the amplitude transformer is used for transmitting ultrasonic waves generated by the ultrasonic transducer to the tool head, and the vibration wall is used for reflecting the ultrasonic waves generated by the ultrasonic transducer.
Preferably, the ultrasonic waves are reflected at a vibrating wall within the tool head and generate a radial resonant standing wave, the vibrating wall of the tool head being located at an antinode of the resonant standing wave.
Preferably, the radius of the vibrating wall r and the frequency of the ultrasonic wave f satisfy the following relationship:
Figure BDA0002529448180000031
wherein f is the frequency of the ultrasonic waves, r is the radius of the vibrating wall, c is the sound velocity in the tool head, σ is the Poisson constant, and Jn is the Bessel function of the Nth class.
Preferably, the vibrating wall is an outer side wall of the tool head, a spiral groove is formed in the outer side wall, and the fluid pipeline is arranged in the spiral groove.
Preferably, the tool head comprises a body and a conduit rack arranged on the body, the fluid conduit being arranged on the conduit rack, the vibrating wall being an outer side wall of the body.
Preferably, the pipe rack comprises a sleeve sleeved on the body, the sleeve is provided with a spirally arranged pore channel, and the pore channel forms the fluid pipeline.
Preferably, the pipe rack includes a plurality of support pieces arranged at intervals in a circumferential direction of the body, the fluid pipes being arranged on the support pieces.
Preferably, the support sheet is provided with a plurality of through holes for the fluid pipeline to pass through, and the through holes are arranged at intervals along the axial direction of the body.
Preferably, the perforations are arranged in at least two rows at intervals in the radial direction of the body.
Preferably, the fluid pipelines are wound and arranged in at least two layers, and medium layers are filled between the fluid pipelines of adjacent layers and between the fluid pipelines and the vibration wall.
Compared with the prior art, the tubular continuous flow ultrasonic reactor provided by the embodiment of the invention has the beneficial effects that: the amplitude transformer is connected with the super-energy heat exchanger and the tool head, ultrasonic waves are transmitted to the tool head by the aid of the amplitude transformer, the ultrasonic waves are totally reflected at a vibration wall of the tool head, reflected waves and excitation waves are superposed, resonance standing waves are formed along the radial direction of the tool head, an antinode is the position where the amplitude of the resonance standing waves is maximum, the vibration wall is arranged at the antinode, the fluid pipeline is wound and arranged on the vibration wall, and energy of the ultrasonic waves can be radiated from the vibration wall and conducted into the fluid pipeline; the surface area of the vibrating wall is large, so that more fluid pipelines can be contacted, the volume of the fluid pipeline can be larger, and the ultrasonic reactor with large volume can be conveniently manufactured; in addition, the ultrasonic transducer is separated from the fluid pipeline through the amplitude transformer, so that the temperature rise caused by heat entering the fluid pipeline can be reduced, and the ultrasonic transducer can be independently cooled.
Drawings
FIG. 1 is a schematic structural view of example 1 of a tubular continuous flow ultrasonic reactor of the present invention;
FIG. 2 is a schematic structural view of example 1 of a tubular continuous flow ultrasonic reactor of the present invention;
FIG. 3 is a schematic structural view of example 3 of a tubular continuous flow ultrasonic reactor of the present invention;
FIG. 4 is a schematic structural view of example 4 of a tubular continuous flow ultrasonic reactor of the present invention;
FIG. 5 is a schematic structural view of a support sheet of the tubular continuous flow ultrasound reactor of FIG. 4.
In the figure, 1, an ultrasonic transducer; 2. an amplitude transformer; 3. a tool head; 31. a body; 32. a sleeve; 321. a duct; 33. a support sheet; 331. perforating; 34. a helical groove; 4. a fluid conduit.
Detailed Description
The following detailed description of embodiments of the present invention is provided in connection with the accompanying drawings and examples. The following examples are intended to illustrate the invention but are not intended to limit the scope of the invention.
Embodiment 1 of a tubular continuous flow ultrasonic reactor according to the present invention, as shown in fig. 1, the tubular continuous flow ultrasonic reactor includes an ultrasonic transducer 1, a horn 22, a tool head 3, and a fluid conduit 4, wherein one end of the horn 22 is connected to the ultrasonic transducer 1, the other end is connected to the tool head 3, the tool head 3 and the horn 22 are tightly connected to the ultrasonic transducer 1 by bolts, and the fluid conduit 4 is wound around an outer sidewall of the tool head 3.
The ultrasonic transducer 1 is used for converting input electric power into mechanical power (i.e. ultrasonic waves) and then transmitting the mechanical power, and the ultrasonic transducer 1 may be any one of a piezoelectric transducer, an electrostatic transducer (a capacitive transducer), a magnetostrictive transducer, an electromagnetic transducer and a mechanical transducer, and is most preferably a piezoelectric transducer, particularly a sandwich type piezoelectric transducer. The operating frequency of the ultrasonic transducer 1 is generally in the interval 18 khz to 500 khz; the power may range from tens of watts to several kilowatts.
The horn 22 is used to transmit ultrasonic waves from the ultrasonic transducer 1 into the tool head 3, exciting the tool head 3 to generate ultrasonic resonance. The horn 22 may be formed of a single cylinder or a plurality of solid cylinders of different diameters, and the material is mainly metal or alloy, such as one or more of aluminum, aluminum alloy, titanium alloy, copper, etc.
The outer side wall of the tool head 3 forms a vibration wall for totally reflecting ultrasonic waves, the ultrasonic waves are totally reflected after contacting the outer side wall in the tool head 3, the reflected waves and the excitation waves are superposed and form resonance standing waves along the radial direction of the tool head 3, the outer side wall is located at the position of an antinode of the resonance standing waves, the ultrasonic vibration at the position of the antinode of the resonance standing waves is strongest, and the fluid pipeline 4 is in contact with the outer side wall, so that the ultrasonic waves can be conveniently and efficiently transmitted into fluid inside the fluid pipeline 4.
The tool head 3 is a solid cylinder structure, and the material of the tool head 3 is mainly metal or alloy, such as aluminum, aluminum alloy, titanium alloy, copper, and the like. The cross section of the tool head 3 is circular, and in order to generate a resonant standing wave in the radial direction of the ultrasonic wave in the tool head 3, the following relation is satisfied between the radius of the tool head 3 and the frequency of the ultrasonic wave:
Figure BDA0002529448180000051
where f is The frequency of The ultrasonic waves, r is The radius of The tool head 3, c is The speed of sound in The tool head 3, σ is The Poisson constant (Poisson ratio, The ratio of The transverse strain to The longitudinal strain of a material when The material is subjected to tensile or compressive forces) of The material used in The tool head, and Jn is a Bessel function of The N-th class, which is common in engineering mathematics (reference GS Field, The residual radial strains of a cylinder of wall thickness, Canadian Journal of research, 1939, 17a (7): 141-. The tool head 3 may also be a cylindrical structure with a cross section of a regular polyhedron, and the equivalent diameter of the tool head 3 and the frequency of the ultrasonic wave satisfy the above relationship.
The fluid conduit 4 is a pipe with a circular cross section, in other embodiments, the cross section of the fluid conduit 4 may also be other shapes, such as a square, a polygon, etc., the equivalent diameter of the cross section of the fluid conduit 4 is 0.5-500 mm, and the material of the fluid conduit 4 may be a plastic polymer (such as ptfe PFA), or may be glass, metal, alloy, composite material, etc. The fluid pipe 4 is wound on the outer side wall of the tool head 3 to increase the contact area of the tool head 3 and the pipe, and the transmission efficiency of ultrasonic waves is increased.
The fluid pipeline 4 is wound and arranged with three layers on the outer side wall of the tool head 3, the medium layers are filled between the adjacent two layers of fluid pipelines 4 and between the innermost fluid pipeline 4 and the outer side wall of the tool head 3, the medium layers are used for increasing the contact area between the fluid pipelines 4 and the tool head 3, and the ultrasonic waves are transmitted to the fluid pipelines 4 from the tool head 3 conveniently.
In embodiment 1, the ultrasonic transducer 1 is a sandwich type ultrasonic transducer 1 of 22 khz, and the ultrasonic transducer 1 has a diameter of 50mm and a length of 90 mm. The length of the amplitude transformer 22 is 220mm, and the amplitude transformer is composed of a plurality of sections of cylinders with different diameters from 37mm to 80mm, and is made of aluminum alloy. The tool head 3 is a cylindrical body 31 with the diameter of 144mm and the height of 55mm, and the material of the body 31 is titanium alloy. The fluid pipe 4 is a glass tube with an outer diameter of 4mm and an inner diameter of 3 mm. The glass tube is wound on the outer side wall of the body 31 for three layers, wherein the first layer is tightly wound for 12 circles, the second layer is wound for 11 circles, and the third layer is wound for 10 circles. The total length of the glass tube was 17m, and the volume was about 120 mL. Epoxy resin glue is filled between the outer side wall of the body 31 and the glass tube and between the glass tube and the glass tube to enhance the contact of the glass tube and the glass tube, so that the propagation of ultrasonic waves is facilitated.
The embodiment 2 of the tubular continuous flow ultrasonic reactor of the present invention, as shown in fig. 2, is different from the embodiment 1 in that a spiral groove 34 is formed on the outer side wall of the tool head 3, the number of the spiral groove 34 is 12, the spiral groove 34 is a semicircular groove with a diameter of 4mm, and the fluid pipe 4 is wound and arranged in the spiral groove 34. The fluid pipe 4 is a glass pipe having an outer diameter of 4mm and an inner diameter of 3 mm. The glass tube is wound with a first layer on the outer side wall of the tool head 3 along the spiral groove 34, and then a second layer is wound on the first layer of glass tube; the first layer is tightly wound for 12 turns, and the second layer is tightly wound for 11 turns. The total length of the glass tube was 11m, and the volume was about 80 mL. Epoxy resin glue is filled between the outer side wall of the tool head 3 and the glass tube and between the glass tube and the glass tube to enhance the contact of the glass tube and the glass tube, so that the transmission of ultrasound is facilitated.
Embodiment 3 of the tubular continuous flow ultrasonic reactor of the present invention, as shown in fig. 3, is different from embodiment 1 in that the tool head 3 includes a body 31 and a pipe rack provided outside the body 31 for arranging fluid pipes. The pipe rack is a sleeve 32 sleeved outside the body 31, the structure of the body 31 is the same as that of the body 31 of the tool head 3 in embodiment 1, the inner diameter of the sleeve 32 is 144mm, the outer diameter is 153mm, the height is 55mm, and the sleeve is made of glass. The sleeve 32 is provided with channels 321 with a diameter of 5mm, the channels 321 are screwed downwards along the length direction of the sleeve 32, the intervals between the channels 321 are 3mm, the length is 3m, the volume is about 60mL, and the channels 321 form a fluid pipeline. Epoxy resin glue is filled between the outer side wall of the body 31 and the sleeve 32 to enhance the contact between the sleeve 32 and the body 31, which is beneficial to the propagation of ultrasonic waves.
Embodiment 4 of the tubular continuous flow ultrasonic reactor of the present invention, as shown in fig. 4 and 5, differs from embodiment 3 in that the tube frame is a support sheet 33 disposed outside the body 31, the support sheets 33 are eight and are arranged at intervals along the circumference of the body 31, and the interval between two adjacent support sheets 33 is 45 degrees. The support sheet 33 is a thin plate with a thickness of 3mm, a width of 20mm and a height of 55mm, two rows of through holes 331 are formed in the support sheet 33, the through holes 331 are used for the fluid pipe 4 to pass through, and the two rows of through holes 331 are arranged at intervals along the radial direction of the body 31. Defining the through holes 331 near the body 31 as a first row of through holes 331, and defining the through holes 331 far from the body 31 as a second row of through holes 331, wherein the first row of through holes 331 is 4mm wide and 11mm high, and 3 in total; the second row of perforations 331 has a circular cross-section with a diameter of 4mm, for a total of 6. The fluid pipeline 4 is a stainless steel pipe, the outer diameter of the stainless steel pipe is 4mm, the inner diameter of the stainless steel pipe is 2.8mm, the stainless steel pipe 1 is wound for 6 circles along the first row of through holes 331 of the supporting sheet 33, and each through hole 331 is wound for two circles; then continue to wind 6 turns along the second row of perforations 331; and finally wound for 12 turns along the outer wall of the support piece 33. The total length of the stainless steel tube was 12m, and the volume was about 85 mL.
To sum up, the embodiment of the present invention provides a tubular continuous flow ultrasonic reactor, wherein an amplitude transformer is connected to a super-energy heat exchanger and a tool head, the amplitude transformer is utilized to transmit ultrasonic waves to the tool head, the ultrasonic waves are totally reflected at a vibration wall of the tool head, reflected waves are superposed with excitation waves, a resonant standing wave is formed along a radial direction of the tool head, an antinode is a position where an amplitude of the resonant standing wave is maximum, the vibration wall is arranged at the position of the antinode, a fluid pipeline is wound and arranged on the vibration wall, and energy of the ultrasonic waves can be radiated from the vibration wall and conducted into the fluid pipeline; the surface area of the vibrating wall is large, so that more fluid pipelines can be contacted, the volume of the fluid pipeline can be larger, and the ultrasonic reactor with large volume can be conveniently manufactured; in addition, the ultrasonic transducer is separated from the fluid pipeline through the amplitude transformer, so that the temperature rise caused by heat entering the fluid pipeline can be reduced, and the ultrasonic transducer can be independently cooled.
The above description is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and substitutions can be made without departing from the technical principle of the present invention, and these modifications and substitutions should also be regarded as the protection scope of the present invention.

Claims (10)

1. A tubular continuous flow ultrasonic reactor is characterized by comprising an ultrasonic transducer, an amplitude transformer, a tool head and a fluid pipeline, wherein one end of the amplitude transformer is connected with the ultrasonic transducer, the other end of the amplitude transformer is connected with the tool head, the fluid pipeline is wound and arranged on a vibration wall of the tool head, the amplitude transformer is used for transmitting ultrasonic waves generated by the ultrasonic transducer to the tool head, and the vibration wall is used for reflecting the ultrasonic waves generated by the ultrasonic transducer.
2. The tubular continuous-flow ultrasound reactor according to claim 1, wherein the ultrasound waves are reflected at a vibrating wall within the tool head and create a radial resonant standing wave, the vibrating wall of the tool head being located at an antinode of the resonant standing wave.
3. The tubular continuous-flow ultrasonic reactor of claim 2, wherein the radius r of the vibrating wall and the frequency f of the ultrasonic waves satisfy the following relationship:
Figure FDA0002529448170000011
Wherein f is the frequency of the ultrasonic waves, r is the radius of the vibrating wall, c is the sound velocity in the tool head, σ is the Poisson constant, and Jn is the Bessel function of the Nth class.
4. The tubular continuous-flow ultrasonic reactor of claim 1, wherein the vibrating wall is an outer sidewall of the tool head, the outer sidewall having a helical groove therein, the fluid conduit being disposed within the helical groove.
5. The tubular continuous-flow ultrasound reactor according to claim 1, wherein the tool head comprises a body and a conduit rack arranged on the body, the fluid conduit being arranged on the conduit rack, the vibrating wall being an outer sidewall of the body.
6. The tubular continuous flow ultrasound reactor according to claim 5, wherein the conduit frame comprises a sleeve fitted over the body, the sleeve having a plurality of helically disposed openings defining the fluid conduit.
7. The tubular continuous-flow ultrasound reactor according to claim 5, wherein the tube rack comprises a plurality of support plates arranged at intervals along a circumference of the body, the fluid tubes being arranged on the support plates.
8. The tubular continuous-flow ultrasonic reactor according to claim 7, wherein the support plate is perforated with a plurality of perforations for the fluid conduit to pass through, the perforations being spaced apart from each other in the axial direction of the body.
9. The tubular continuous-flow ultrasound reactor according to claim 8, wherein the perforations are arranged in at least two rows spaced radially of the body.
10. The tubular continuous flow ultrasound reactor according to any of claims 1 to 9, wherein the fluid conduits are arranged in a winding of at least two layers, with a layer of medium filled between the fluid conduits of adjacent layers and between the fluid conduits and the vibrating wall.
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CN113731326A (en) * 2021-08-19 2021-12-03 化学与精细化工广东省实验室 Large-volume ultrasonic tubular reactor
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Application publication date: 20201030