CN115254222A - Method for preparing monodisperse non-Newtonian fluid droplets based on asymmetric parallel micro-channels - Google Patents
Method for preparing monodisperse non-Newtonian fluid droplets based on asymmetric parallel micro-channels Download PDFInfo
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01L—CHEMICAL OR PHYSICAL LABORATORY APPARATUS FOR GENERAL USE
- B01L3/00—Containers or dishes for laboratory use, e.g. laboratory glassware; Droppers
- B01L3/02—Burettes; Pipettes
- B01L3/0241—Drop counters; Drop formers
- B01L3/0265—Drop counters; Drop formers using valves to interrupt or meter fluid flow, e.g. using solenoids or metering valves
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01L—CHEMICAL OR PHYSICAL LABORATORY APPARATUS FOR GENERAL USE
- B01L3/00—Containers or dishes for laboratory use, e.g. laboratory glassware; Droppers
- B01L3/50—Containers for the purpose of retaining a material to be analysed, e.g. test tubes
- B01L3/502—Containers for the purpose of retaining a material to be analysed, e.g. test tubes with fluid transport, e.g. in multi-compartment structures
- B01L3/5027—Containers for the purpose of retaining a material to be analysed, e.g. test tubes with fluid transport, e.g. in multi-compartment structures by integrated microfluidic structures, i.e. dimensions of channels and chambers are such that surface tension forces are important, e.g. lab-on-a-chip
- B01L3/502769—Containers for the purpose of retaining a material to be analysed, e.g. test tubes with fluid transport, e.g. in multi-compartment structures by integrated microfluidic structures, i.e. dimensions of channels and chambers are such that surface tension forces are important, e.g. lab-on-a-chip characterised by multiphase flow arrangements
- B01L3/502784—Containers for the purpose of retaining a material to be analysed, e.g. test tubes with fluid transport, e.g. in multi-compartment structures by integrated microfluidic structures, i.e. dimensions of channels and chambers are such that surface tension forces are important, e.g. lab-on-a-chip characterised by multiphase flow arrangements specially adapted for droplet or plug flow, e.g. digital microfluidics
Abstract
The invention discloses a method for preparing monodisperse non-Newtonian fluid droplets based on asymmetric parallel microchannels, and belongs to the technical field of micro chemical engineering. The microchannel device consists of an upper cover plate and a bottom plate, wherein the upper cover plate is provided with a two-phase liquid inlet hole and a liquid outlet communicated to the bottom plate of the microchannel. The lower bottom plate consists of a fluid distribution pipe, parallel branches, two T-shaped junctions and a liquid drop collection pipe. The method for preparing the monodisperse non-Newtonian fluid droplets based on the asymmetric parallel microchannel improves the production efficiency of droplet preparation, can conveniently realize the regulation and control of droplet size through two-phase flow change, and has good stability and uniform droplet size in the droplet preparation process. Has wide application value in the fields of fine chemical engineering, biological medicine, materials, food and the like.
Description
Technical Field
The invention belongs to the technical field of micro chemical engineering, and particularly relates to a method for preparing monodisperse non-Newtonian fluid droplets based on an asymmetric parallel microchannel device.
Background
The micro-droplets can provide relatively independent micro-reaction, micro-mixing and micro-separation spaces for the fields of chemical reaction, biosynthesis, material preparation and the like. The droplet size is a necessary condition to ensure efficient performance of the corresponding process. The traditional methods for preparing micro-droplets mainly comprise a mechanical stirring method and a membrane emulsification method, but the methods consume large amounts of reagents, and the prepared micro-droplets have poor monodispersity and are unstable. The fine chemical technology has the excellent characteristic of precise control, which makes the fine chemical technology have absolute advantages in preparing uniform liquid drops. However, the production throughput of the single-pipeline micro-channel is small, and the mass preparation of micro-droplets is severely restricted. Patent CN107511189B discloses a preparation method of monodisperse micro-droplets based on capillary, which has small production flux and can not realize continuous preparation. The micro-channel device for preparing monodisperse non-Newtonian fluid micro-droplets by using acoustic radiation in the patent CN114160218A also has only a single pipeline, and the problem of small production flux is also existed.
In the amplification process, the distribution condition of the fluid flow in the parallel pipelines influences the size uniformity of the liquid drops, and even the liquid drops cannot be generated when the cross flow occurs. In addition, the flowing medium used in the microchannel usually contains high molecular substances, etc., and the fluid has complex nonlinear fluid rheological characteristics in the flowing process, such as the fluid viscosity and elasticity are closely related to the deformation rate, thus the fluid distribution and the monodispersity of the liquid drops are seriously influenced. Therefore, high-throughput preparation of uniform micro-droplets based on parallel amplification is one of the important concerns. Patent CN113304790A discloses a microchannel basic unit and array set thereof for realizing high-throughput preparation of micro-droplets. The basic unit of the focusing device is a structure similar to a Chinese character hui shape and provided with two focusing structures, the structure is complex, and the requirements on processing and manufacturing are high.
Current parallel microchannels can be structurally divided into symmetric parallel microchannels and asymmetric parallel microchannels. The patent CN110624616A adopts a three-dimensional tree-shaped symmetric parallel amplification method to increase the yield of micro droplets, and the difference in the processing precision of the pipeline and the roughness of the surface of the pipeline in the micro-channel will cause uneven distribution of the fluid, and the space utilization rate is low. The asymmetric parallel microchannel has the advantages of strong disturbance resistance, compact arrangement, easy integration, high space utilization rate and the like, and the key point of preparing uniform liquid drops by the asymmetric parallel microchannel lies in reasonable structural layout and size design.
Disclosure of Invention
In order to solve the problems in the prior art, the invention provides a method for preparing monodisperse non-Newtonian fluid droplets based on asymmetric parallel microchannels, which aims to solve the problems of low droplet production efficiency and non-uniform droplet size in the prior art.
The technical scheme of the invention is as follows:
an asymmetric parallel microchannel consists of an upper cover plate and a lower base plate, wherein the upper cover plate is provided with a two-phase liquid inlet and a liquid outlet which are communicated with the lower base plate; the microchannel device body comprises: the device comprises a continuous phase inlet, a parallel channel for transporting a continuous phase fluid, a dispersed phase inlet, a main channel for transporting the dispersed phase fluid, a parallel channel for transporting the dispersed phase fluid, two T-shaped structures, a parallel channel for transporting droplets, a droplet collecting main channel and a droplet discharging port, wherein the continuous phase fluid inlet is connected with the parallel channel for transporting the continuous phase fluid, the dispersed phase fluid inlet is connected with the main channel for transporting the dispersed phase fluid, the main channel is vertically connected with the parallel channel for transporting the dispersed phase fluid, the parallel channel for transporting the continuous phase fluid, the parallel channel for transporting the dispersed phase fluid and the parallel channel for transporting the droplets are connected through the T-shaped structures, the other end of the parallel channel for transporting the droplets is vertically connected with the droplet collecting main channel, and a liquid discharging port is positioned at the tail end of the droplet collecting main channel.
The parallel channels for transporting the continuous phase fluid have the same length, the length is 50-100 times of the height of the micro-channel, the height of the micro-channel is 50-1000 μm, and the width-to-height ratio is 0.1-10.
The liquid inlet of the dispersed phase is positioned at one side of the micro-channel, the width of the main channel for transporting the dispersed phase fluid is 1-30 times of the height of the micro-channel, and the lengths of the parallel channels for transporting the dispersed phase fluid are the same and 10-20 times of the height of the micro-channel.
The width of the main droplet collecting channel is 1-30 times the height of the microchannel, and the droplet discharging port is located on the opposite side of the inlet side of the dispersed phase, both of which are zigzag.
The number of the parallel channels for transporting the dispersed phase fluid is consistent with that of the parallel channels for transporting the continuous phase fluid, and the specific number is set according to requirements and is more than or equal to 2.
A method for preparing monodisperse non-Newtonian fluid droplets based on asymmetric parallel microchannels is characterized in that a continuous phase and a disperse phase are respectively injected into the asymmetric parallel microchannels from a continuous phase inlet and a disperse phase inlet, the two immiscible phases are contacted at a T-shaped structure, the disperse phase generates droplets under the action of continuous phase extrusion force and shearing force, and then the droplets are discharged out of the microchannels through a liquid discharge port, and the droplets with different sizes are prepared by two-phase flow regulation.
The continuous phase is one of organic solvents of cyclohexane, n-butane, paraffin oil and silicone oil.
The dispersed phase is one of aqueous solutions of sodium carboxymethylcellulose, xanthan gum, polyethylene oxide and polyacrylamide or polyethylene glycol solutions added with nano silicon dioxide, the addition concentration of macromolecules in the aqueous solution is 0.003-4%, and the concentration of silicon dioxide with the particle size of 15nm added in the polyethylene glycol is 5-15%.
The continuous phase or the disperse phase contains one of surfactants Span40, span80, span85, tween 20 and Tween 80, and the addition amount of the surfactant is 2-7%.
The invention has the following beneficial effects:
the device and the method of the invention complete the preparation of uniform non-Newtonian fluid droplets, can realize the continuous preparation of droplets with different sizes by two-phase flow regulation and control, and have accurate control and simple and convenient operation. By arranging the asymmetric parallel micro pipelines, the preparation efficiency of liquid drops is improved, the disturbance resistance of a system is enhanced, the space utilization rate of a micro-channel chip is improved, the material cost is reduced, and the processing and the manufacturing are convenient. The droplets prepared in both lines are of good uniformity. The production flux of the microchannel basic unit can be further improved by the array arrangement of the microchannel basic unit.
Drawings
FIG. 1 is a schematic diagram of a microchannel structure according to the present invention;
wherein: 1-a continuous phase inlet; 2-parallel channels transporting continuous phase fluid; 3-dispersed phase inlet; 4-a main channel for transporting the dispersed phase fluid; 5-parallel channels for transporting the dispersed phase fluid; 6-T type structure; 7-parallel channels transporting droplets; 8-a droplet collection main channel; 9-a liquid discharge port;
in FIG. 2, (a), (b) and (c) are Qd=60 μ L/min, dispersed phase flow QcRespectively 200 mu L/min,300 mu L/min and 400 mu L/min to prepare uniform non-Newtonian liquid drops with different sizes;
FIG. 3 is a diagram showing a droplet size distribution prepared at a dispersed phase injection flow rate of 60. Mu.L/min and a dispersed phase injection flow rate of 200. Mu.L/min using the present microchannel.
The specific implementation mode is as follows:
the following provides a detailed description of the method for preparing monodisperse non-Newtonian droplets based on asymmetric parallel microchannels in the present invention with reference to the accompanying drawings and examples.
Example 1:
at normal temperature, preparing polyacrylamide and deionized water according to the mass ratio of 1. And (3) fully mixing the surfactant span85 and cyclohexane according to a mass ratio of 5. The width of the main channel for transporting the dispersed phase is 20 times of the height, and the width-to-height ratio of other pipelines is 1. Injecting a continuous phase and a disperse phase from inlets 1 and 3 of the micro-channel respectively, wherein the injection flow rate of the disperse phase is 50 mu L/min, and the injection flow rate of the continuous phase is 800 mu L/min. After the two are met at the T-shaped junction, under the action of extrusion force and shearing force of continuous phase fluid, non-Newtonian liquid drops with the diameter of 480 mu m are generated, and the generated liquid drops flow out of the microchannel from the discharge port and enter the collecting device.
Example 2:
at normal temperature, sodium carboxymethylcellulose and deionized water are prepared according to the mass ratio of 1. And (3) fully mixing the surfactant span85 and cyclohexane according to a mass ratio of 5. The width-height ratio of the main channel for transporting the dispersed phase and the main channel for collecting the liquid drops is 20, and the width-height ratio of other pipelines is 1. The continuous phase and the dispersed phase were injected from the inlets 1 and 3 of the microchannel, respectively, with the injection flow rate of the dispersed phase being 250. Mu.L/min and the injection flow rate of the continuous phase being 200. Mu.L/min. After the two meet at the T-shaped junction, under the action of extrusion force and shearing force of continuous phase fluid, non-Newtonian liquid drops with the diameter of 740 mu m are generated, and the generated liquid drops flow out of the micro-channel from the discharge port and enter the collecting device.
Example 3:
at normal temperature, sodium carboxymethylcellulose and deionized water are prepared according to the mass ratio of 0.1. And (3) fully mixing the surfactant span85 and cyclohexane according to a mass ratio of 5. The width-to-height ratio of the main droplet collecting channel was 20, and the width-to-height ratios of the other tubes were all 1. The continuous phase and the dispersed phase are injected from the inlets 1 and 3 of the microchannel respectively, the injection flow rate of the dispersed phase is 20 muL/min, and the injection flow rate of the continuous phase is 400 muL/min. After the two meet at the T-shaped junction, under the action of extrusion force and shearing force of continuous phase fluid, non-Newtonian liquid drops with the diameter of 520 μm are generated, and the generated liquid drops flow out of the microchannel from the discharge port and enter the collecting device.
Example 4:
at normal temperature, preparing polyacrylamide and deionized water according to the mass ratio of 1. And (3) fully mixing the surfactant span85 and cyclohexane according to a mass ratio of 5. The width to height ratio of all the tubes in the microchannel is 1. The continuous phase and the dispersed phase were injected from the inlets 1 and 3 of the microchannel, respectively, with the injection flow rate of the dispersed phase being 250. Mu.L/min and the injection flow rate of the continuous phase being 400. Mu.L/min. After the two meet at the T-shaped junction, under the action of extrusion force and shearing force of continuous phase fluid, non-Newtonian liquid drops with the diameter of 600 μm are generated, and the generated liquid drops flow out of the microchannel from the discharge port and enter the collecting device.
Example 5:
at normal temperature, preparing polyacrylamide and deionized water according to a mass ratio of 0.3. And (3) fully mixing the surfactant span85 and cyclohexane according to a mass ratio of 5. The width-to-height ratio of the main droplet collecting channel was 20, and the width-to-height ratios of the other tubes were all 1. And injecting a continuous phase and a disperse phase from inlets 1 and 3 of the micro-channel respectively, wherein the injection flow rate of the disperse phase is 350 mu L/min, and the injection flow rate of the continuous phase is 400 mu L/min. After the two meet at the T-shaped junction, under the action of extrusion force and shearing force of continuous phase fluid, non-Newtonian liquid drops with the diameter of 616 mu m are generated, and the generated liquid drops flow out of the microchannel from the discharge port and enter the collecting device.
Example 6:
preparing the silica nanoparticles and polyethylene glycol according to a mass ratio of 8 to 100, adding 4% of tween-20, and fully stirring to fully mix the silica particles and the polyethylene glycol to prepare a dispersed phase. The continuous phase is silicone oil with viscosity of 10 mPas. The width-to-height ratio of the main droplet collecting channel was 20, and the width-to-height ratios of the other tubes were all 1. Injecting a continuous phase and a disperse phase from inlets 1 and 3 of the micro-channel respectively, wherein the injection flow rate of the disperse phase is 40 mu L/min, and the injection flow rate of the continuous phase is 50 mu L/min. After the two meet at the T-shaped junction, under the action of extrusion force and shearing force of continuous phase fluid, non-Newtonian liquid drops with the diameter of 500 mu m are generated, and the generated liquid drops flow out of the microchannel from the discharge port and enter the collecting device.
Example 7:
preparing the silica nanoparticles and polyethylene glycol according to a mass ratio of 10 to 100, adding 4% of tween-20, and fully stirring to fully mix the silica particles and the polyethylene glycol to prepare a dispersed phase. The continuous phase is silicone oil with viscosity of 10 mPas. The width-to-height ratio of the main droplet collecting channel was 20, and the width-to-height ratios of the other tubes were all 1. Injecting a continuous phase and a disperse phase from inlets 1 and 3 of the micro-channel respectively, wherein the injection flow rate of the disperse phase is 10 mu L/min, and the injection flow rate of the continuous phase is 50 mu L/min. After the two meet at the T-shaped junction, under the action of extrusion force and shearing force of continuous phase fluid, non-Newtonian liquid drops with the diameter of 385 mu m are generated, and the generated liquid drops flow out of the micro-channel from the discharge port and enter a collecting device.
The above description is only an example of the present invention and is not intended to limit the present invention in any manner. Any simple modification, replacement, or improvement made by those skilled in the relevant art according to the technical spirit of the present invention still falls within the scope of the technical solution of the present invention.
Claims (9)
1. An asymmetric parallel microchannel is characterized by comprising an upper cover plate and a lower base plate, wherein the upper cover plate is provided with a two-phase liquid inlet and a liquid outlet which are communicated with the lower base plate; the microchannel device body includes: the device comprises a continuous phase inlet (1), a parallel channel (2) for transporting a continuous phase fluid, a dispersed phase inlet (3), a main channel (4) for transporting a dispersed phase fluid, a parallel channel (5) for transporting a dispersed phase fluid, two T-shaped structures (6), a parallel channel (7) for transporting liquid drops, a liquid drop collection main channel (8) and a liquid drop discharge port (9); the continuous phase fluid inlet (1) is connected with a parallel channel (2) for transporting continuous phase fluid, the dispersed phase fluid inlet (3) is connected with a main channel (4) for transporting dispersed phase fluid, the main channel (4) is vertically connected with a parallel channel (5) for transporting dispersed phase fluid, the parallel channel (2) for transporting continuous phase fluid, the parallel channel (4) for transporting dispersed phase fluid and the parallel channel (7) for transporting liquid drops are connected through a T-shaped structure (6), the other end of the parallel channel (7) for transporting liquid drops is vertically connected with a main liquid drop collecting channel (8), and a liquid discharge port (9) is positioned at the tail end of the main liquid drop collecting channel (8).
2. The asymmetric parallel microchannel according to claim 1, wherein the parallel channels (2) transporting the continuous phase fluid have the same length, the length being 50 to 100 times the height of the microchannel, the height of the microchannel being 50 to 1000 μm, and the aspect ratio being 0.1 to 10.
3. The asymmetric parallel microchannel of claim 1, wherein the dispersed phase inlet is located at one side of the microchannel, the width of the main channel (4) transporting the dispersed phase fluid is 1-30 times the height of the microchannel, and the length of the parallel channel (5) transporting the dispersed phase fluid is the same and 10-20 times the height of the microchannel.
4. The asymmetric parallel microchannel according to claim 1, wherein the droplet collecting main channel (8) has a width 1 to 30 times as large as the height of the microchannel, and the droplet discharging port (9) is located on the opposite side of the inlet side of the dispersed phase, and both are zigzag-shaped.
5. The asymmetric parallel microchannel of claim 1, wherein the number of parallel channels for transporting the dispersed phase fluid is equal to or greater than 2, and the number of parallel channels for transporting the continuous phase fluid is set according to the requirement.
6. A method for preparing monodisperse non-Newtonian fluid droplets based on an asymmetric parallel microchannel is characterized in that a continuous phase and a disperse phase are respectively injected into the asymmetric parallel microchannel according to any one of claims 1 to 5 from a continuous phase inlet (1) and a disperse phase inlet (3), the immiscible two phases are contacted at a T-shaped structure (6), the disperse phase generates droplets under the action of continuous phase extrusion force and shearing force, and then the droplets are discharged from the microchannel through a liquid discharge port (9), and droplets with different sizes are prepared by two-phase flow regulation.
7. The method for preparing monodisperse non-Newtonian fluid droplets based on asymmetric parallel microchannel of claim 6, wherein the continuous phase is one of organic solvent cyclohexane, n-butane, paraffin oil, silicone oil.
8. The method for preparing monodisperse non-Newtonian fluid droplets based on the asymmetric parallel microchannel, which is characterized in that the disperse phase is the aqueous solution of sodium carboxymethylcellulose, xanthan gum, polyethylene oxide and polyacrylamide or the polyethylene glycol solution added with nano silicon dioxide, the addition concentration of macromolecules in the aqueous solution is 0.003% -4%, and the concentration of silicon dioxide with the particle size of 15nm added in the polyethylene glycol is 8% -15%.
9. The method of claim 6, wherein the continuous phase or the dispersed phase contains one of the surfactants Span40, span80, span85, tween 20 and tween 80, and the amount of the surfactant added is 2% to 7%.
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| WO2013014216A1 (en) * | 2011-07-27 | 2013-01-31 | Instytut Chemii Fizycznej Polskiej Akademii Nauk | Device and method for high-throughput, on-demand generation and merging of droplets |
| CN105013547A (en) * | 2015-07-30 | 2015-11-04 | 天津大学 | Novel microbubble/liquid drop generation regulation and control device and novel microbubble/liquid drop generation regulation and control method |
| CN108671970A (en) * | 2018-04-11 | 2018-10-19 | 华南师范大学 | A kind of production method of double size microlayer models based on micro-fluidic chip |
| KR102043161B1 (en) * | 2018-06-07 | 2019-11-11 | 한양대학교 산학협력단 | Microfluidic Device for Merging Micro-droplets and Method for Merging Micro-droplets Using Same |
| CN110052298A (en) * | 2019-05-09 | 2019-07-26 | 中国计量大学 | A method of vibration pipeline control micro-fluidic chip generates microlayer model |
| CN110624616A (en) * | 2019-10-28 | 2019-12-31 | 西安交通大学 | Three-dimensional microfluidic device and method for high-throughput micro-droplet generation |
| CN114160218A (en) * | 2021-11-15 | 2022-03-11 | 大连理工大学 | Microfluidic device and method for preparing monodisperse non-Newtonian micro-droplets |
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