CN104162395B - Method for enhancing gas-liquid process in micro-reactor - Google Patents
Method for enhancing gas-liquid process in micro-reactor Download PDFInfo
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Abstract
The invention relates to a method for enhancing a gas-liquid process in a micro-reactor. The method comprises the following steps: applying ultrasound of a specific frequency to a gas-liquid micro-reactor in which gas liquid two-phase flow is bubble flow, slug flow, slug annular flow, stirring flow or annular flow; and regulating and controlling the transverse equivalent diameter of a gas phase in the gas-liquid two-phase flow and the ultrasonic frequency till a product of the ultrasonic frequency and the transverse equivalent diameter of the gas phase is up to 1-40 mm.kHz. According to the method, disturbance and acoustic streaming are caused in liquid by using the ultrasound and the cavitation effect of the gas phase, so that gas-liquid mass transfer is enhanced; and meanwhile, agglomeration between a solid or a sticky substance in fluid or the adhesion to the wall surface of a micro channel can be broken, so that blockage is prevented and dredged. The method for enhancing the gas-liquid process disclosed by the invention is suitable for the fields of various gas-liquid reactions, gas absorption, gas separation and purification, and the like.
Description
Technical field
The invention belongs to the field such as chemical process intensifying method, chemical industry equipment, applications of ultrasound, specifically a kind of utilization
Gas-liquid mass transfer, the method simultaneously preventing from blocking in ultrasound-enhanced microchannel.
Background technology
Microreactor refers to the chemical industry equipment in a few micrometers to several millimeters yardstick for the inner structural features size.This internal junction
Structure is commonly referred to as microchannel.With respect to traditional gas-liquid contactor or reactor, such as stirred tank, bubble tower, falling liquid film contact
Device etc., gas-liquid microreactor has that specific surface is high, heat and mass speed is fast, safe operation, be easy to amplify, to take up an area space little etc. excellent
Point.Therefore gas-liquid microreactor has wide practical use in fields such as gas liquid reaction, GAS ABSORPTION, gas isolation of purified.
But gas-liquid microreaction technology there is also some shortcomings.Microchannel size in microreactor is little, therefore easy quilt
Impurity or process fluid blocking, particularly when processing containing solid or generating solid or the very big fluid of viscosity.In addition,
Because microchannel size is little, flowing is generally in laminar condition and surface tension effects are notable, makes gas-liquid mass transfer in microchannel
Strengthening is relatively difficult.
At present, in microchannel, microchannel is mainly designed to the knot such as bending, obstacle, collision by the intensifying method of gas-liquid process
Structure is strengthening the relative motion of gas-liquid, and is causing vortex to strengthen mass transfer in local.(j.tan, the mass transfer such as j.tan
performance of gas–liquid segmented flow in microchannels,chemical
Engineering journal181 182 (2012) 229 235) by microchannel design in the arc-shaped strengthening gas-liquid mass transfer, send out
Existing radius of curvature is that the microchannel of 10mm improves 2-3 times relative to straight channel mass tranfer coefficient.maría jose nieves
(mar í a jose nieves-remacha, the gas-liquid flow and mass transfer in an such as remacha
Advanced-flow reactor, ind.eng.chem.res.2013,52,8996-9010) to test Corning Incorporated special
The microreactor of the heart-shaped structure described in sharp pct101873890a strengthens the result of gas-liquid mass transfer, finds gas Liquid Mass Transfer Coefficient ratio
The high an order of magnitude of traditional stirred tank.
The above by microchannel be designed to bend the structure such as obstacle to strengthen the method for gas-liquid mass transfer can in some occasions
To reach reasonable result.But the method is typically only applicable to the higher occasion of velocity ratio, the mass transfer effect when velocity ratio is relatively low
Really poor.Microchannel is made to be easier to block in addition, microchannel is designed to the structures such as bending obstacle.
Content of the invention
In order to solve the above problems, present inventor has performed further investigation.Find: if applied in gas-liquid microreactor
Ultrasonic, using ultrasonic and gas phase cavitation, make gas liquid film high vibration and the motion in microchannel, and in a liquid
Cause disturbance and acoustic streaming, so as to efficient hardening gas-liquid mass transfer.The ultrasonic sound intensity of input is bigger, and gas-liquid mass transfer effect is better.Gas
Liquid mass transfer effect mainly to be controlled by sound intensity size, no matter in high flow rate or low flow velocity, can reach very strong mass transfer effect
Really.In addition, the vibration of microchannel wall and disturbance caused by gas liquid film high vibration under ultrasonication, can destroy in fluid
Gathering between solid or dope and solid or dope, in the adhesion of microchannel wall, are blocked up such that it is able to preventing and dredging
Plug.Therefore, this method flow velocity scope of application width using ultrasound-enhanced gas-liquid process, can efficient hardening mass transfer, can also prevent
Stop and dredge the blocking of microchannel.
The present invention is based on the studies above and parses proposition technical scheme below:
Apply the ultrasonic of characteristic frequency in gas-liquid microreactor, the gas liquid film making gas-liquid two-phase in microchannel is super
The lower heavy vibratory movements of acoustic cavitation effect.Wherein, gas-liquid two-phase manifold is chosen as bubble flow, slug flow, plays shape annular flow, stirring
One of stream and annular flow.
In described gas-liquid microreactor, gas phase in gas-liquid two-phase manifold, its horizontal equivalent diameter is 10-5000 μ
m；The supersonic frequency applying is 16-600khz.Supersonic frequency f is f*d=1- with the matching relationship of gas phase horizontal equivalent diameter d
40mm khz, preferably f*d=4-30mm khz.
Gas-liquid two-phase manifold is a known concept in field of chemical engineering, refers to gas phase shape in liquid phase.Micro-
In reactor, bubble flow, slug flow, bullet shape annular flow, stirring stream and annular flow are modal several gas-liquid two-phase manifolds.
The horizontal equivalent diameter of described gas phase is that in gas-liquid manifold, gas phase is equivalent straight in the section on flow direction
Footpath.When gas-liquid two-phase manifold is bubble flow, section equivalent diameter is the diameter of bubble；Bubble diameter and quantity can be by gas-liquids
Biphase flow velocity is regulating and controlling；When gas-liquid two-phase manifold is slug flow, plays shape annular flow, the section equivalent diameter of gas phase mainly by
The cross sectional dimensions of microchannel are regulating and controlling；When gas-liquid two-phase manifold is stirring stream and annular flow, the lateral cross section of gas phase is equivalent
Diameter is regulated and controled by the cross sectional dimensions of microchannel and the flow velocity of gas-liquid two-phase simultaneously.
In described gas-liquid microreactor, ultrasonic transducer can be bonded in microreactor outer surface, make ultrasonic biography
Lead entrance microreactor；Ultrasonic transducer can also be integrated in inside microreactor, make ultrasonic direct conduction enter microchannel；
Whole microreactor can also be put in ultrasonic cleaning tank.
This method utilizes the ultrasonic cavitation with gas phase, makes gas-liquid interface high vibration and the motion in microchannel, and
Cause disturbance and acoustic streaming in a liquid, so as to efficient hardening gas-liquid mass transfer.The ultrasonic sound intensity of input is bigger, and gas-liquid mass transfer is imitated
Fruit is better.Under certain sound intensity, when supersonic frequency f meets above-mentioned matching relationship with the horizontal minimum dimension of gas phase, ultrasonic
Reach resonance with gas phase, now gas-liquid interface vibrates and most motion intense, the disturbance causing in a liquid and acoustic streaming are the most notable, because
This gas-liquid mass transfer strengthening effect is best.It is higher than or for this matching relationship, ultrasonic and gas phase can not reach resonance, now gas-liquid
Interface vibration and motion are weaker, and strengthening effect is poor.
When this method can be applicable to gas-liquid two-phase manifold for slug flow or annular flow, using frequency 16-600khz and the sound intensity
Higher than 0.5w/cm2The ultrasonic gas-liquid process intensification carrying out GAS ABSORPTION.
When this method can be applicable to gas-liquid two-phase manifold for slug flow, it is higher than 0.5w/ using frequency 16-600khz and the sound intensity
cm2Ultrasonic carry out being related to the strengthening of the gas-liquid reaction process of solid.
This method can apply to the strengthening of various gas absorption process, the such as gas such as carbon dioxide, sulfur dioxide
Physical Absorption, MODEL OF CHEMICAL ABSORPTION PROCESS.Various gas-liquid chemical reaction processes, the more particularly to reaction of solid can also be applied to
Journey.The so-called course of reaction being related to solid, has referred to that solid participates in reaction as reactant, catalyst etc., or has generated in product
Some is the course of reaction of solid.
The present invention under slug flow and annular flow, by applying frequency 20 KHz ultrasonic it is seen that gas Liquid Mass Transfer Coefficient
Improve about 9 times, GAS ABSORPTION rate is greatly improved.The present invention can be also used for strengthening the gas liquid reaction being related to solid, Ke Yiyou
Effect prevents and dredge blockage.
Brief description
Fig. 1 is the MCA schematic diagram used by all embodiments of the invention.Wherein, 1 is liquid inlet channel, and 2 are
Gas entrance passage, 3 is main channel.
Fig. 2 is the change in pressure drop curve of microchannel in the embodiment of the present invention 3.
Specific embodiment
To further illustrate the present invention below by embodiment.
Microreactor involved by following all embodiments is single channel microreactor, and MCA is as shown in Figure 1.Figure
In 1,1 be liquid inlet channel, 2 be gas entrance passage, both be deeply all 1000 μm, wide 500 μm.3 is main channel, i.e. gas-liquid
Process channel, deep 1000 μm wide 1000 μm of main channel, length 90mm.
Embodiment 1 gas-liquid physical absorption process is strengthened
The present embodiment is taking utilize ultrasound-enhanced physical absorption process as a example in gas-liquid microreactor.Liquid in microchannel
Access road 1 is passed through deionized water, and flow is 2ml/min, is passed through pure carbon dioxide, flow is in gas entrance passage 2
1.65ml/min.As shown in Fig. 2 the gas being passed through forms continuous slug flow, the horizontal equivalent diameter of bubble in main channel 3
About 1000 μm.Not plus ultrasonic when, because carbon dioxide is by the absorption of water, absorbance is 26.7%.When 20 kilo hertzs of operating frequency of applying
Hereby, sound intensity 1.5w/cm2Ultrasonic when, gas-liquid mass transfer is accelerated, and the absorbance of carbon dioxide is 56.3%.Can be counted according to Mass Transfer Model
Calculate gas-liquid cumulative volume mass tranfer coefficient, when finding not add ultrasonic, overall mass transfer coefficient is 0.10s-1, plus ultrasonic rear overall mass transfer coefficient increase
To 0.87s-1, improve about 9 times.It can be seen that the ultrasonic strengthening effect to Gas-Liquid Slug Flow mass transfer is obvious.
Embodiment 2 gas-liquid MODEL OF CHEMICAL ABSORPTION PROCESS is strengthened
The present embodiment is taking utilize ultrasound-enhanced MODEL OF CHEMICAL ABSORPTION PROCESS as a example in gas-liquid microreactor.Liquid in microchannel
Access road 1 is passed through monoethanolamine mea(molecular formula nh of mass fraction 20%2ch2ch2Oh) solution, flow 1ml/min, in gas
It is passed through 10% carbon dioxide (Balance Air is nitrogen), flow 20ml/min, the gas being passed through is main logical in body access road 2
Form annular flow, about 900 μm of the cross-sectional diameter of gas phase in road 3.After gas and mea solution are passed through main channel 3, contact with each other biography
Concurrently biochemical reaction makes carbon dioxide be absorbed by mea solution chemistry to matter.The material that reactor outlet the has reacted gas commonly used
Liquid knockout drum carries out gas-liquid separation, and the concentration with gas analyzer for CO2 measurement carbon dioxide in gas, then can calculate dioxy
Change the absorbance of carbon.Not plus ultrasonic when, carbon dioxide absorption rate be 55.1%.When applying operating frequency 18 KHz, the sound intensity
1.5w/cm2Ultrasonic when, absorbance brings up to 89.3%.It can be seen that ultrasound-enhanced gas-liquid mass transfer effect is obvious.
Embodiment 3, the gas-liquid reaction process strengthening of generation solid
The present embodiment is taking utilize the gas-liquid reaction process of ultrasound-enhanced generation solid as a example in gas-liquid microreactor.Micro-
The liquid inlet channel 1 of passage is passed through the (nh that mass fraction is 5%4)2sif6Solution, flow 10ml/min, leads in gas access
It is passed through pure nh in road 23Gas, flow 10ml/min.(nh4)2sif6Solution and nh3After gas is passed through main channel 3, is formed and play shape
Stream, and the mass transfer that contacts with each other, generation chemical reaction generate Silica solids granule.Not plus ultrasonic when, the oxygen generating in main channel 3
SiClx solids particles precipitate is in channel wall, and over time is cumulative, and pressure drop is gradually increased therewith.After about 15 minutes
Passage 3 blocks, and pressure drop is increased to 0.95mpa(and sees Fig. 2), reactor outlet does not have fluid to flow out.Now, apply frequency to reactor
Rate 25 KHz, the sound intensity are 1.5w/cm2Ultrasonic, the pressure drop of reactor drops to 0.03mpa immediately, and reactor outlet is immediately
Fluid is had to flow out.In the presence of this is ultrasonic, reactor continuously runs 5 hours and has no obvious pressure oscillation, and pressure exists always
0.03-0.05mpa.It can be seen that the method really can effectively be prevented and be dredged microchannel blocking.
Claims (3)
1. a kind of method strengthening gas-liquid process in microreactor, in gas-liquid microreactor, applying characteristic frequency is ultrasonic, makes micro-
In passage the boundary of gas-liquid two-phase under ultrasonic cavitation heavy vibratory movements it is characterised in that: gas-liquid two-phase manifold is
Slug flow or annular flow, are higher than 0.5w/cm using frequency 16-600khz and the sound intensity2The ultrasonic gas-liquid mistake carrying out GAS ABSORPTION
Cheng Qianghua, the gas phase in gas-liquid two-phase manifold, its horizontal equivalent diameter is 10-5000 μm；The supersonic frequency applying is 16-
600khz；Supersonic frequency f is f*d=1-40mm khz with the matching relationship of gas phase horizontal equivalent diameter d.
2. method according to claim 1 it is characterised in that: described apply in gas-liquid microreactor ultrasonic, surpass
The matching relationship of acoustic frequency f and gas phase horizontal equivalent diameter d is f*d=4-30mm khz.
3. according to the arbitrary described method of claim 1～2 it is characterised in that: gas-liquid two-phase manifold be slug flow, using frequency
16-600khz and the sound intensity are higher than 0.5w/cm2Ultrasonic carry out being related to the strengthening of the gas-liquid reaction process of solid.
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| CN108264448B (en) * | 2017-01-03 | 2019-08-06 | 万华化学集团股份有限公司 | A kind of reaction system preparing bata-phenethyl alcohol, catalyst and its process |
| CN108499147A (en) * | 2017-02-28 | 2018-09-07 | 中国石油化工股份有限公司 | Distributed ultrasound bubble column rectifier unit in parallel and method |
| CN108970559B (en) * | 2018-09-18 | 2023-10-27 | 云南民族大学 | Manufacturing method of ultrasonic reinforced solid-liquid micro-reaction device |
| CN109020811A (en) * | 2018-09-19 | 2018-12-18 | 张家港瀚康化工有限公司 | The method for preparing propionic ester using microreactor |
| CN113003851A (en) * | 2020-11-13 | 2021-06-22 | 四川全息生态环境技术产业有限公司 | Ultrasonic, ozone and micro-channel advanced oxidation method and device thereof |
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