阅读说明：本技术 一种超声强化撞击流反应系统及其工艺方法 (Ultrasonic reinforced impinging stream reaction system and process method thereof ) 是由 曾宏伟 陈律名 于 2021-10-13 设计创作，主要内容包括：本发明公开一种超声强化撞击流反应系统,包括第一反应液原液桶、第二反应液原液桶、产物桶、蠕动泵、可见光分光光度计、超声波发生装置、泰勒反应器和撞击流反应器；所述撞击流反应器的下端两侧分别设有第一进口和第二进口,下方为出口,第一反应液原液桶通过蠕动泵与第一进口连接,第二反应液原液桶通过蠕动泵与第二进口连接,超声变幅杆的一端从撞击流反应器的上端插入,另一端与超声波发生装置连接,反应器出口与泰勒反应器连接,然后通入产物桶与可见光分光光度计连接。本发明超声的引入可以对撞击滞流区产生一个强扰动,有效改善撞击流反应器内的混合效果,达到强化反应的作用。同时引入泰勒反应器,对于反应的传质有很好的强化作用。(The invention discloses an ultrasonic-enhanced impinging stream reaction system, which comprises a first reaction liquid stock solution barrel, a second reaction liquid stock solution barrel, a product barrel, a peristaltic pump, a visible spectrophotometer, an ultrasonic generating device, a Taylor reactor and an impinging stream reactor; the two sides of the lower end of the impinging stream reactor are respectively provided with a first inlet and a second inlet, an outlet is arranged below the impinging stream reactor, a first reaction liquid stock solution barrel is connected with the first inlet through a peristaltic pump, a second reaction liquid stock solution barrel is connected with the second inlet through the peristaltic pump, one end of an ultrasonic amplitude transformer is inserted from the upper end of the impinging stream reactor, the other end of the ultrasonic amplitude transformer is connected with an ultrasonic generating device, the outlet of the reactor is connected with a Taylor reactor, and then the ultrasonic amplitude transformer is introduced into a product barrel to be connected with a visible light spectrophotometer. The introduction of the ultrasonic wave can generate strong disturbance to the impact stagnant zone, effectively improve the mixing effect in the impact flow reactor and achieve the effect of enhancing the reaction. Meanwhile, the Taylor reactor is introduced, so that the mass transfer of the reaction is well enhanced.)

1. An ultrasonic-enhanced impinging stream reaction system is characterized by comprising a first reaction liquid stock solution barrel (1), a second reaction liquid stock solution barrel (2), a product barrel (3), a peristaltic pump (4), a visible light spectrophotometer (6), an ultrasonic wave generating device (7), an ultrasonic amplitude transformer (8), a Taylor reactor (9) and an impinging stream reactor (13); the device is characterized in that a first inlet (10) and a second inlet (11) are respectively arranged on two sides of the lower end of the impinging stream reactor (13), an outlet (12) of the reactor is arranged below the impinging stream reactor (13), a first reaction liquid stock solution barrel (1) is connected with the first inlet (10) through a peristaltic pump (4), a second reaction liquid stock solution barrel (2) is connected with the second inlet (11) through the peristaltic pump (4), one end of an ultrasonic amplitude transformer (8) is inserted into the impinging stream reactor (13) from the upper end of the impinging stream reactor (13), the other end of the ultrasonic amplitude transformer is connected with an ultrasonic wave generating device (7), the outlet (12) of the impinging stream reactor (13) is connected with a Taylor reactor (9), and the outlet of the Taylor reactor (9) is communicated into a product barrel (3).

2. An ultrasonically enhanced impinging stream reaction system according to claim 1, wherein the outlet of the product barrel (3) is further connected with a visible light spectrophotometer (6) for detecting the concentration of the target product in the product.

3. An ultrasonically enhanced impinging stream reaction system according to claim 2, wherein the pressure gauge (5) is arranged at the connection of the first inlet (10) and the peristaltic pump (4), the connection of the second inlet (11) and the peristaltic pump (4), and the outlet (12).

4. An ultrasound-enhanced impinging stream reaction system according to claim 1, wherein a fixing structure is provided above the inside of the impinging stream reactor (13) for fixing the ultrasound horn (8).

5. An ultrasonically enhanced impinging stream reaction system according to claim 1, wherein an electric motor is arranged above the taylor reactor (9), and the type and power of the electric motor are selected according to requirements.

6. A process of ultrasonically enhanced impinging stream reaction systems according to any one of claims 1 to 5, comprising the steps of:

(1) preparing required acid and alkali reaction stock solution, and placing the required acid and alkali reaction stock solution in a first reaction solution stock solution barrel (1) and a second reaction solution stock solution barrel (2);

(2) turning on the ultrasonic wave generating device (7), and setting the ultrasonic output power of the ultrasonic wave generating device (7);

(3) adjusting the flow of the peristaltic pump (4) according to the required Reynolds number Re;

(4) opening two peristaltic pumps (4) to enable the acid-base reaction liquid to generate impact reaction in the middle part of the impact flow reactor;

(5) simultaneously, the rotating speed of the motor of the Taylor reactor (9) is adjusted according to the required speed;

(6) after the flow is stable, taking out the product from the product barrel (3), and detecting the concentration of the target product in the product by using a visible light spectrophotometer (6);

(7) and (4) carrying out a plurality of experiments according to different Reynolds numbers Re, and measuring the concentration value of the target product in the required product.

Technical Field

The invention belongs to the field of reactor development and chemical fluid mechanics, and particularly relates to an ultrasonic-enhanced impinging stream reaction system and a process method thereof.

Background

Since the advent of the impinging stream reactor, the impinging stream reactor has been widely used in industrial processes such as mixing, liquid phase extraction, absorption and desorption, preparation of ultrafine powders and nanomaterials due to its good transfer characteristics and excellent mixing effect, wherein the flow and mixing have an important influence on the precipitation and crystallization reactions in the reactor.

However, in the conventional impinging stream reaction, an obvious stagnant zone (as shown in fig. 3) is formed at the upper end of the impinging zone, which results in insufficient impinging stream reaction, and thus the particle size of the reaction product is relatively large, and the product performance in some application fields requiring a relatively high particle size of the product, such as in some catalyst and ultrafine powder preparation fields, is not high, so that the application of the impinging stream reactor is limited to a certain extent, and therefore, a device for enhancing the mixing effect and reaction degree of reactants in the impinging stream reactor and improving the product performance is urgently needed to be developed. In recent years, process intensification has been increasingly emphasized, and therefore, researchers in various countries have been developing and researching various reactors to intensify the transfer process, and the development and research are becoming hot spots of research.

Disclosure of Invention

Aiming at the problems in the prior art, the invention provides an ultrasonic-enhanced impinging stream reaction system and a process method thereof, wherein the reaction system further enhances the micromixing performance by introducing an ultrasonic field and a Taylor reactor into an impinging stream reactor.

In order to achieve the purpose, the invention adopts the following technical scheme:

an ultrasonic intensified impinging stream reaction system comprises a first reaction liquid stock solution barrel, a second reaction liquid stock solution barrel, a product barrel, a peristaltic pump, a visible light spectrophotometer, an ultrasonic wave generating device, an ultrasonic amplitude transformer, a Taylor reactor and an impinging stream reactor; the device comprises an impinging stream reactor, a first reaction liquid raw liquid barrel, a second reaction liquid raw liquid barrel, an ultrasonic amplitude transformer, a product barrel and a visible light spectrophotometer, wherein a first inlet and a second inlet are respectively arranged on two sides of the lower end of the impinging stream reactor, an outlet of the impinging stream reactor is arranged below the impinging stream reactor, the first reaction liquid raw liquid barrel is connected with the first inlet through a peristaltic pump, the second reaction liquid raw liquid barrel is connected with the second inlet through the peristaltic pump, one end of the ultrasonic amplitude transformer is inserted into the impinging stream reactor from the upper end of the impinging stream reactor, the other end of the ultrasonic amplitude transformer is connected with an ultrasonic wave generating device, the outlet of the ultrasonic amplitude transformer is connected with the Taylor reactor, and the outlet of the Taylor reactor is communicated with the product barrel and is connected with the visible light spectrophotometer.

Further, a fixing structure is arranged above the inside of the impinging stream reactor and used for fixing the ultrasonic amplitude transformer.

Furthermore, pressure gauges are arranged at the joint of the first inlet and the peristaltic pump, the joint of the second inlet and the peristaltic pump and the outlet.

Furthermore, a motor which can be equipped according to requirements is arranged above the Taylor reactor, and the type of the motor is selected according to the requirements.

The invention also provides a process method of the ultrasonic reinforced impinging stream reaction system, which mainly comprises the following steps:

(1) preparing needed acid and alkali reaction stock solution, and placing the required acid and alkali reaction stock solution in a first reaction solution stock solution barrel and a second reaction solution stock solution barrel;

(2) turning on the ultrasonic wave generating device, and setting the ultrasonic output power of the ultrasonic wave generating device;

(3) adjusting the flow of the peristaltic pump according to the Reynolds number Re required;

(4) opening two peristaltic pumps to enable the acid-base reaction liquid to generate impact reaction in the middle of the impact flow reactor;

(5) simultaneously, the rotating speed of a motor of the Taylor reactor is adjusted according to the required speed;

(6) after the flow is stable, taking out the product from the product barrel, and detecting the concentration of the target product in the product by using a visible spectrophotometer;

(7) and (4) carrying out multiple experiments according to different Reynolds numbers Re, and measuring the concentration value of the required product.

The invention adopts ultrasound to improve the micro-mixing formation of the impinging stream reactor, and the advantages of high penetrability, high energy density, convenient process, safety, reliability and the like of the ultrasound are regarded as excellent means for improving the mixing and mass transfer performance in the microreactor, and the ultrasonic cavitation effect is mainly used for generating violent acoustic current vortex to the surrounding flow field when the cavitation bubble vibrates (stable cavitation) or collapses (transient cavitation) to generate turbulent motion of fluid so as to strengthen the mixing and mass transfer.

When the ultrasonic action is combined with the impinging stream reactor, the mixing effect in the impinging stream reactor can be further enhanced due to the cavitation effect of the ultrasonic, so that the product is better. The most obvious effect is that the particle diameter of the superfine powder is smaller, and the specific surface area of the superfine powder can be improved when the catalyst material is prepared.

And taylor reactors are a class of reactors made based on the taylor vortex principle. Between two coaxial cylinders rotating relatively (usually, the inner cylinder rotates and the outer cylinder is stationary), when the inner circular rotation speed is higher than a certain critical speed, the centrifugal force will induce a series of circular vortexes (i.e. taylor vortexes) arranged alternately and orderly along the cylinder axis, as shown in fig. 4, and the secondary flow stronger than the flow along the rotating body of the rotating shaft is called taylor flow. Taylor reactors have been used in chemical, biological, and material fields in recent years, and have been developed in a wide variety of ways. Taylor reactors have a number of advantages over conventional reactors. When the reactor operates in a laminar flow Taylor flow state, the medium flow in the Taylor reactor is close to ideal plug flow; the Taylor reactor can simultaneously ensure higher mass transfer coefficient and smaller shear stress; the taylor reactor can also maintain the uniform fluidization of solid catalyst particles when a heterogeneous reaction is carried out, but unlike in a fluidized bed, the particles are mainly maintained in a suspended state by the taylor vortex action rather than the axial flow action in the taylor reactor, so that even under extremely low axial flow velocity, a good fluidization effect can be obtained by adjusting the rotating speed of the cylinder, and the limit of the lowest axial flow velocity in the fluidized bed is broken through.

Therefore, in order to enhance the performance of precipitation and crystallization in the impinging stream reactor, the invention enhances the micro-mixing performance in the impinging stream reactor by introducing a supersonic field in the impinging stream reactor, and simultaneously introduces a Taylor reactor to enhance mass transfer to further enhance the micro-mixing performance.

The invention has the beneficial effects that: compared with the traditional impinging stream (as shown in figure 3), the invention adopts the two-end fluid impinging area of the ultrasonic intensified impinging stream reactor, and has an obvious stagnant area at the upper end of the impinging area, and the introduction of the ultrasonic wave can effectively generate a strong disturbance in the stagnant area, thereby effectively improving the mixing effect in the impinging stream reactor and achieving the effect of intensifying the reaction. Meanwhile, the Taylor reactor is introduced, so that the mass transfer of the reaction is well enhanced.

Drawings

FIG. 1 is a schematic view of the overall system of the present invention;

FIG. 2 is a schematic diagram of the impinging stream reactor and ultrasonic amplitude rod assembly of the present invention;

FIG. 3 is a velocity vector diagram of a conventional impinging stream;

FIG. 4 is a schematic Taylor flow diagram;

FIG. 5 is a graph comparing the measured ionization indices (with and without sonication) at different Reynolds numbers Re for the examples.

In the figure: 1. a first reaction solution stock solution barrel; 2. a second reaction solution stock solution barrel; 3. a product barrel; 4. a peristaltic pump; 5. a pressure gauge; 6. a visible light spectrophotometer; 7. an ultrasonic wave generating device; 8. an ultrasonic horn; 9. a Taylor reactor; 10. a first inlet; 11. a second inlet; 12. an outlet; 13. impinging stream reactors.

Detailed Description

The invention will be further described with reference to the drawings and examples in the following description, but the scope of the invention is not limited thereto.

As shown in fig. 1 and fig. 2, a set of ultrasonic-enhanced impinging stream reaction system includes a first reaction liquid stock solution barrel 1, a second reaction liquid stock solution barrel 2, a product barrel 3, a peristaltic pump 4, a visible light spectrophotometer 6, an ultrasonic wave generating device 7, an ultrasonic amplitude transformer 8, a taylor reactor 9 and an impinging stream reactor 13; a first reaction liquid stock solution barrel 1 is connected with a first inlet 10 through a peristaltic pump 4, a second reaction liquid stock solution barrel 2 is connected with a second inlet 11 of the impinging stream reactor through the peristaltic pump 4, one end of an ultrasonic amplitude transformer 8 is inserted into the impinging stream reactor from the upper end of the impinging stream reactor, the other end of the ultrasonic amplitude transformer is connected with an ultrasonic generating device 7, an outlet 12 of the impinging stream reactor is connected with a Taylor reactor 9 and then is communicated with a product barrel 3, the product barrel 3 is connected with a visible light spectrophotometer 6, and in addition, pressure gauges 5 are arranged at the connecting part of the first inlet 10 and the peristaltic pump 4, the connecting part of the second inlet 11 and the peristaltic pump 4 and the outlet 12.

FIG. 2 is a schematic view of the assembly of an impinging stream reactor and an ultrasonic horn, the ultrasonic horn functioning as shown in FIG. 2, the front end face of the horn being at the interface area after the entrance to the two ends of the reactor, the front end of the ultrasonic horn vibrating at a higher frequency when the ultrasonic generating means is open. Compared with the traditional device without applying ultrasonic wave (as shown in fig. 3), the high-intensity vibration of the front end can form a strong disturbance at the stagnant zone at the bottom end of the impact area, and the effect of enhancing the reaction can be achieved.

Application example 1

Potassium iodide and iodate parallel competitive reaction system

An application of an ultrasonic-enhanced impinging stream reaction system is disclosed, wherein the reaction system is applied to an iodine reaction system, and the reaction system is a parallel competitive reaction system and consists of the following three steps:

further, wherein the reaction (1) is an acid-base neutralization reaction, which is a transient reaction, and the reaction rate isk₁＝10¹¹L/(mol. s), reaction rate of reaction (2)Wherein k is₂And ionic strength I_sThe following relationships exist:

the reaction rate of the reaction (3) isAt 25 ℃ has

Further, in the case of acid deficiency, the yield of iodine is used as a measure of the micromixing uniformity, and in the case of partial isolation, the yield of iodine, Y, is:

at full isolation, the yield of iodine was:

defining an outlier index X_sCharacterizing the degree of micromixing, then:

ionization index X_sHas a value in the range of 0. ltoreq.X_s1 or less, under optimum conditions (i.e.thorough mixing), X_SThis means that according to the first reaction equation, the acid is instantaneously dispersed and consumed by the borate solution, and the entire solution is a colorless liquid at this timeI₂And I-₃In the worst case (i.e. when completely separated), X is 0_S＝1。

The following steps are adopted in the specific operation of the embodiment:

1. preparing required acid and alkali reaction stock solution, (wherein the acid reaction solution is H with the concentration of 0.05mol/L₂SO₄The solution and the alkali reaction solution are 0.1818mol/L H mol₃BO₃、0.0909mol/LNaOH、0.01167mol/L KI、0.00233mol/L KIO₃Mixed solution) of (a) and (b) are respectively placed in a first reaction solution stock solution barrel 1 and a second reaction solution stock solution barrel 2;

2. adjusting the flow of the peristaltic pump 4 according to the Reynolds number Re required by the user;

3. opening the two peristaltic pumps 4 to enable the acid-base reaction liquid to generate impact in the middle part of the impact flow reactor to react;

4. simultaneously, the rotating speed of the motor of the Taylor reactor 9 is adjusted according to the required speed;

5. after the flow is stable, taking out the product from the product barrel 3, and detecting the concentration of iodine in the product by using a visible light spectrophotometer 6;

6. carrying out multiple experiments according to different Reynolds numbers Re to obtain a concentration value of a required product;

7. the ultrasonic wave generator 7 was turned on, the ultrasonic output power of the ultrasonic wave generator 7 was set, and the 2.3.4.5.6 procedure was repeated to measure the iodine concentration in the product and convert it to an ionization index, and the result is shown in fig. 5.

As can be seen from FIG. 5, under different Reynolds numbers Re, the obtained ionization indexes are lower than those obtained without the application of the ultrasonic field, so that the reaction solution can be mixed more sufficiently under the ultrasonic action to enhance the reaction.