CN113058516A - Preparation method of microfluidic complex liquid drop induced by liquid-liquid phase separation - Google Patents
Preparation method of microfluidic complex liquid drop induced by liquid-liquid phase separation Download PDFInfo
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- CN113058516A CN113058516A CN202110290630.7A CN202110290630A CN113058516A CN 113058516 A CN113058516 A CN 113058516A CN 202110290630 A CN202110290630 A CN 202110290630A CN 113058516 A CN113058516 A CN 113058516A
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Abstract
A method for preparing microfluidic complex droplets induced by liquid-liquid phase separation comprises the following steps: the continuous phase and the disperse phase respectively flow into the microfluidic chip under the pressure driving, uniform single-phase droplets are generated in a droplet forming area, and the single-phase droplets are subjected to liquid-liquid phase separation under the stimulation of physical or chemical factors and gradually evolve into monodisperse complex droplets. The complex liquid drop preparation method induced by liquid-liquid phase separation can avoid complex fluid control, is compatible with the existing liquid drop scale amplification technology, and is beneficial to high-throughput preparation and large-scale application of complex liquid drops.
Description
Technical Field
The invention relates to a method for preparing complex liquid drops by liquid-liquid phase separation induction, belonging to the technical field of microfluidic liquid drops.
Background
The microfluidic droplets are small-volume units formed by a microfluidic chip platform for controlling multiphase fluid, have the characteristics of small volume, good monodispersity, high flux and the like, and show great application potential in the aspects of micro-nano material preparation, biochemical analysis, high-flux screening and the like. With the deep application of the microfluidic droplet technology in the field of functional material synthesis, droplets with a simple spherical structure hardly meet the template requirements of intelligent materials. The preparation of complex droplets with advanced structures is an urgent need, such as Janus droplets, core-shell droplets, multi-core double emulsions, multi-layer droplets, and the like. At present, the preparation of microfluidic complex droplets generally adopts a manifold control method, namely a local patterning technology is adopted to ensure that different regions of a microfluidic chip keep different hydrophilic and hydrophobic characteristics, the movement of multiphase fluid is accurately regulated and controlled by pressure, accurate manifold is formed in the chip, and the complex droplets are formed by one-step or multi-step emulsification. Precise manifold control results in reduced system stability and reduced droplet monodispersity. On the other hand, the complicated manifold needs a plurality of micropumps or a plurality of pressure sources for operation, which leads to a rapid increase in the difficulty of parallel amplification of a plurality of droplet formation units, and is not favorable for droplet scale preparation. The simple one-step preparation of droplets with advanced and complex structures using the two-phase fluid commonly used for chip droplets still remains a challenge. Based on the above, the idea of combining the microfluidic droplet technology and the liquid-liquid phase separation technology is provided, and the problem of scale preparation of complex droplets is expected to be solved.
Disclosure of Invention
The invention aims to provide a method for preparing a microfluidic complex droplet by liquid-liquid phase separation induction, which adopts two-phase fluid commonly used for chip droplets to prepare the complex droplet with a high-grade structure in one step and is beneficial to the large-scale preparation of the microfluidic complex droplet.
In order to realize the aim, the invention provides a method for preparing microfluidic complex droplets by liquid-liquid phase separation induction. The continuous phase and the dispersed phase respectively flow into the microfluidic chip under the pressure driving, uniform single-phase droplets are generated in a droplet forming area, and the single-phase droplets are subjected to liquid-liquid phase separation under the stimulation of physical or chemical factors and gradually evolve into monodisperse complex droplets.
Further, the continuous phase is one or a mixture of more of hydrogen carbon oil and fluorocarbon oil.
Further, the dispersed phase is a binary or multi-element miscible system.
Further, the pressure drive is one or a combination of a peristaltic pump, a syringe pump, air pressure, hydraulic pressure and gravity.
Furthermore, the material of the microfluidic chip is one or a combination of more of polydimethylsiloxane, polycarbonate, polymethyl methacrylate, polystyrene, polyethylene terephthalate, polyamide, epoxy resin and polyurethane.
Further, the monodispersity is that the variation coefficient of the droplet size is between 0.1% and 15%.
Further, the composition distribution of the single phase droplets may be uniform or non-uniform.
Further, the physical factors are one or more of volatilization, diffusion and temperature change.
Further, the chemical factor is a combination of one or more chemical reactions.
Further, the complex liquid drop is one or a plurality of shape compounds of Janus liquid drops, core-shell liquid drops, multi-core liquid drops and multilayer liquid drops.
Compared with the prior art, the invention has the beneficial technical effects that:
the method combines the micro-fluidic droplet technology with the liquid-liquid phase separation process, utilizes the common two-phase fluid control of chip droplets to prepare the complex droplets with high-grade structures in one step, ensures the monodispersity of the complex droplets, is easy to couple with the droplet scale amplification technology, is favorable for improving the productivity of the complex droplets, and shows better application prospects in the fields of intelligent materials, food storage and the like.
Drawings
FIG. 1 volatilization induced liquid-liquid phase separation to produce Janus droplets;
fig. 2 evaporation-induced liquid-liquid phase separation to prepare Janus droplets with higher structure, 1 for core-shell Janus droplets, 2 for triple Janus droplets, and 3 for multiple Janus droplets;
FIG. 3 temperature-induced liquid-liquid phase separation to prepare a double emulsion with reversible configuration, 1 for homogeneous droplets and 2 for double emulsion;
figure 4 topography control of the double emulsion.
The specific implementation mode is as follows:
the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Example 1 volatilization-induced liquid-liquid phase separation for the preparation of monodisperse Janus droplets
A ternary mixture of water, n-octanol and ethyl acetate was used as a dispersed phase, fluorocarbon oil (FC40) containing 2% of surfactant was used as a continuous phase, and homogeneous droplets were formed on a chip (visual based droplet control in negative pressure driver generator for large-scale particle synthesis, Handin Li, et al. electrophoresis 2017,38, 1736-. Since FC40 has good gas permeability, ethyl acetate in the homogeneous droplets volatilizes into the external environment, water and n-octanol undergo phase separation, and the homogeneous droplets eventually evolve into Janus droplets (fig. 1). The proportion of water and n-octanol in the dispersed phase is changed, the proportion of the water part and the n-octanol part of the Janus liquid drop is changed, and the appearance of the Janus liquid drop is adjusted. When the ternary mixture system is upgraded to the quaternary mixture system, the Janus droplet configuration is upgraded, and a higher-level and more complex structure can be formed (figure 2). Taking a quaternary blending system of NOA61, n-octanol, water and ethyl acetate as a dispersion phase, and inducing liquid-liquid phase separation to form a core-shell Janus droplet along with volatilization of a cosolvent ethyl acetate; taking a quaternary blending system of NOA61, hexadecane, water and acetone as a disperse phase, and inducing liquid-liquid phase separation to form a triple Janus droplet along with volatilization of a cosolvent acetone; a quaternary blending system of NOA61, liquid paraffin, water and ethyl acetate is used as a disperse phase, and liquid-liquid phase separation is induced to form multiple Janus droplets along with volatilization of a cosolvent ethyl acetate.
Example 2 temperature-induced liquid-liquid phase separation for configurationally reversible monodisperse double emulsion Synthesis
A binary mixture of water and ionic liquid is used as a disperse phase, fluorocarbon oil (FC40) containing 2% of surfactant is used as a continuous phase, and homogeneous liquid drops are formed on a chip with a T-channel structure. The electrical heating causes the temperature of the system to rise. When the temperature of the homogeneous phase liquid drop is higher than the critical phase transition temperature of the ionic liquid, liquid-liquid phase separation occurs in the liquid drop, and the ionic liquid component and the water component are gradually converged and separated to form monodisperse double emulsion. The system is gradually cooled, the ionic liquid part and the water part are gradually fused, and the double emulsions return to homogeneous liquid drops. The configuration of the liquid drop is controlled by temperature from homogeneous phase to core-shell structure, and has reversibility (figure 3). The proportion of water and ionic liquid in the dispersed phase is changed, and the proportion of the water part and the ionic liquid part of the double emulsion is changed, so that the adjustment of the size of the inner core and the thickness of the shell is realized. The variation of the ratio of water to ionic liquid did not affect the monodispersity of the double emulsion, the uniformity of the core, and the consistency of the shell thickness (figure 4).
Claims (10)
1. A method for preparing microfluidic complex droplets by liquid-liquid phase separation induction is characterized by comprising the following steps:
(1) respectively enabling the continuous phase and the dispersed phase to flow into the microfluidic chip under the pressure driving, and generating monodisperse single-phase droplets in a droplet forming area;
(2) under the stimulation of physical or chemical factors, the single-phase liquid drops gradually evolve into monodisperse complex liquid drops.
2. The method for preparing the microfluidic complex droplet induced by liquid-liquid phase separation according to claim 1, wherein the continuous phase is one or a mixture of hydrogen carbon oil and fluorocarbon oil.
3. The method for preparing microfluidic complex droplets induced by liquid-liquid phase separation according to claim 1, wherein the dispersed phase is a binary or multicomponent miscible system.
4. The method for preparing the microfluidic complex droplet induced by liquid-liquid phase separation according to claim 1, wherein the pressure driving manner is one or a combination of a peristaltic pump, a syringe pump, air pressure, hydraulic pressure and gravity.
5. The method for preparing a microfluidic complex droplet by liquid-liquid phase separation induction according to claim 1, wherein the microfluidic chip is made of one or more of polydimethylsiloxane, polycarbonate, polymethyl methacrylate, polystyrene, polyethylene terephthalate, polyamide, epoxy resin and polyurethane.
6. The method for preparing microfluidic complex droplets induced by liquid-liquid phase separation according to claim 1, wherein the monodispersity is that the variation coefficient of droplet size is between 0.1% and 15%.
7. The method for preparing microfluidic complex droplets induced by liquid-liquid phase separation according to claim 1, wherein the distribution of the components of the single-phase droplets can be uniform or non-uniform.
8. The method for preparing the microfluidic complex droplet induced by liquid-liquid phase separation according to claim 1, wherein the physical factors are one or more of volatilization, diffusion and temperature change.
9. The method for preparing microfluidic complex droplets induced by liquid-liquid phase separation according to claim 1, wherein the chemical factor is the recombination of one or more chemical reactions.
10. The method for preparing the microfluidic complex droplet induced by liquid-liquid phase separation according to claim 1, wherein the complex droplet is one or more of a Janus droplet, a core-shell droplet, a multi-core droplet and a multilayer droplet.
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| CN102941050A (en) * | 2012-11-22 | 2013-02-27 | 清华大学 | Method for preparing even and hollow liquid drops based on micro-fluidic technology |
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2021
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| CN102941050A (en) * | 2012-11-22 | 2013-02-27 | 清华大学 | Method for preparing even and hollow liquid drops based on micro-fluidic technology |
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