KR101229257B1 - Method of making film microreactor with 3-dimensional multilayered microchannel - Google Patents

Abstract

The present invention relates to a method for manufacturing a film-type micro-reactor formed with chemically, thermally and mechanically stable three-dimensional multilayer microchannels through a production process and a simple process. In this case, a three-dimensional microchannel or a three-dimensional multilayer structure may be formed by a single bonding process.
The film-type micro-reactor having a three-dimensional multi-layer microchannel manufactured by the present invention has a flexible feature, and can increase the yield by including a larger amount of microchannels than a conventional microreactor per unit thickness. In addition to being able to continuously react a series of reactions, it is possible to recycle the reaction to provide a variety of three-dimensional micro-reactor applications.

Description

Method of making film microreactor with 3-dimensional multilayered microchannel

The present invention relates to a method for producing a film type micro-reactor consisting of multiple layers of three-dimensional microchannels.

A micro reactor is a micro-channel formed by processing a channel of several microns in size, and refers to a reactor capable of mixing the fluid while passing through the flow channel and discharging the mixed fluid. Materials used to make microreactors include silicon, glass, polymers and the like, including metals. The fabrication of such microreactors ranges from methods derived from electronics to micro-etching techniques to the latest ultra-precision process technologies, and semiconductor processes using dry or wet etching of silicon and glass are mainly utilized. The materials such as metal, silicon, and glass are the best materials for producing high quality micro reactors based on the excellent mechanical strength and high reliability of the material itself in MEMS technology and Lab-on-a-chip technology derived therefrom. Although it has been spotlighted, due to problems such as low moldability and high cost of processing, it has become a factor to increase the manufacturing cost of the micro reactor. In addition, polymer materials such as polymethylmethacrylate (PMMA) and polydimethylsiloxane (PDMS) are easily manufactured due to low process cost and simple manufacturing process, while being resistant to organic solvents and thermally stable. This low limits the operating conditions of the microreactor. Therefore, for a wide range of applications of microreactors, there is a need for the development of microreactors that are chemically, thermally, and mechanically stable than conventional polymer materials, and that can be easily manufactured in a lower cost and simpler process than high reliability materials such as silicon and glass.

On the other hand, the application range of the micro-reactor having a three-dimensional microchannel has been used in various ways, such as a droplet microdevice, a micro valve system, a micro mixer. When two or more fluids pass through a microchannel in a conventional two-dimensional microchannel, a long microchannel necessary for mixing is required due to the formation of a low Reynolds number laminar flow, and to solve this problem, a micro-etching technique and a multilayer photolithography technique are used. Research has been reported to include a micromixer structure having a complex shape inside a microchannel or to manufacture a microchannel having a three-dimensional structure having a flow in a vertical direction to an existing two-dimensional microchannel. There are many reports on the technology of manufacturing a micromixer structure, but the method is made through a complicated process of high cost or has a disadvantage of low moldability and long manufacturing time, and the multi-layered photolithography technique is widely used. The inherent properties of dimethylsiloxanes limit their application. Therefore, there is a need for a research on manufacturing a micro-reactor having three-dimensional microchannels that can be easily and quickly manufactured and is thermally, chemically and mechanically stable.

The present invention is to provide a micro-reactor for producing a micro-reactor, chemically, thermally, mechanically stable and to reduce the production cost by producing a film-type micro-reactor consisting of a three-dimensional multilayer microchannel by a simple process.

The conventional production of two-dimensional and three-dimensional microchannels is a factor to increase the manufacturing cost of the micro-reactor due to problems such as low formability, high cost processing and complex processes, polymethylmethacrylate (PMMA), Polymeric materials such as polydimethylsiloxane (PDMS) are limited in the operating conditions of the microreactor due to low resistance to organic solvents and low thermal stability.

In order to solve the above problems, the present invention aims to quickly and easily make a film-type micro-reactor consisting of chemically, thermally and mechanically stable three-dimensional multilayer microchannels in a low cost simple process. Chemical, thermal, and mechanically stable microchannels can be expected to be applied to a variety of microreactors, and the multilayered film-type microreactors with three-dimensional microchannels can be used to produce more than conventional microreactors per unit thickness. Including positive microchannels allows for increased production in microreactors.

The present invention has been made in order to achieve the above object, it is possible to reduce the production cost and mass production through a simple process of a film-type micro-reactor consisting of three-dimensional multi-layer microchannel chemically, thermally, mechanically stable.

Hereinafter, the present invention will be described in more detail.

The present invention comprises the steps of: (a) etching the polymer film to form at least one microchannel: (b) laminating at least three polymer films on which at least one channel is formed using metal pins; And (c) provides a method for producing a film-type micro-reactor having a three-dimensional multilayer microchannels of three or more laminated polymer film through a one-step multilayered bonding process.

The polymer film of step (a) is formed by etching a fluid inlet, a microchannel portion through which the fluid flows, or a fluid discharge portion through which the introduced fluid is discharged using a laser.

The polymer film is polyimide, polyethylene, polyethylene, fluorinated ethylene propylene, polypropylene, polyethylene terephthalate, polyethylene naphthalate, or polysulfone polysulfone).

At this time, the polymer film is a film of 10 ~ 200 ㎛ thickness depending on the purpose of use of the same or different types of polymer film.

In addition, the microchannel of step (a) is characterized in that the etching by adjusting the depth of the microchannel according to the purpose of use at a ratio of 1/5 ~ 1 of the polymer film thickness.

Stacking of the step (b) is characterized in that to form a hole in the same position on the corner of each of the polymer film in which the microchannel is formed and fixed using a metal pin. When etching the polymer film using a laser, microchannels are formed in each polymer film according to a drawing designed to form three-dimensional microchannels through lamination, and holes of 1 mm diameter are located at the same corner positions of each polymer film. By forming and stacking four places, the predesigned three-dimensional structure is maintained.

Preferably, the lamination is performed by laminating and fixing by using a metal pin having a diameter of 1 mm in the same hole formed in each of the three or more polymer films etched with a laser.

The single bonding step of step (c) is characterized in that the laminated film is integrally bonded by heating and pressing at a temperature of the glass transition temperature (T _g ) to the melting point of the polymer film.

When laminating the polymer film of the step (b) comprises the step of further laminating a release layer film having a melting point lower than the temperature used in the bonding process at the top and the bottom. The method may further include laminating a polymer film having a melting point higher than the temperature used in the bonding process between the reinforcing film and the polymer film in which the microchannels are etched. This is useful for improving the adhesion to bond three or more polymer films integrally.

The reinforcement film melted by heat during the single bonding process by laminating a polymer film having a melting point higher than the temperature used in the bonding process at the top and the bottom by the above lamination between the reinforcement film and the polymer film etched with at least one channel. It can be prevented from entering into the microchannel of the film. In addition, the thermoplastic polymer film having a melting point lower than the temperature used in the bonding process is laminated as a release layer film to remove bubbles formed at the interface of the polymer films by recording the reinforcement film by temperature during a single bonding process. Done.

The reinforcement film laminated in addition to the bonding process removes bubbles formed at the interface of the polymer films to improve pressure resistance, thereby manufacturing a film-type micro-reactor having three-dimensional multilayer microchannels which is advantageous for high velocity and gas phase reactions. .

The film type micro-reactor according to the present invention is characterized in that the total inflow rate is 1 ~ 5000 μl / min when one or more fluids are introduced into the reactor due to the additional reinforcement film laminated in the bonding process.

The film-type microreactor according to the present invention is characterized by having a multi-layered multi-channel structure by performing a single bonding process of three or more laminated polymer films. As a result, the bonding process may be simplified to stack three or more polymer films etched by one or more channels to form a multilayer channel structure by a single bonding process.

Through the multi-layer stacking of the film type micro-reactor in which the three-dimensional microchannels are formed, the amount of microchannels may be increased in a microreactor including a larger amount of microchannels than a conventional microreactor per unit thickness.

The multi-layer film-type micro-reactor of the three-dimensional microchannel manufactured by the present invention has the advantage of obtaining a larger amount of reaction products than the conventional two-dimensional channel by having a multilayer structure.

When manufacturing a multilayer film type micro reactor having a microchannel having a three-dimensional structure in the above, it can be expected to use a variety of micro reactor by using a polymer film that is chemically, thermally, mechanically stable.

Reacting by introducing one or more fluids into the micro reactor includes performing one or more reactions.

The reaction can be expected not only to continuously react a series of reactions, but also to various recycling reactors by enabling a recycling reaction.

By using a thermoplastic polymer film having a thickness of 25 to 200 μm as a material of the microreactor in the present invention, the manufactured multi-layered film type microreactor having a three-dimensional microchannel has excellent solubility and has a flexible feature.

The present invention relates to a method for manufacturing a film-type micro-reactor formed with chemically, thermally and mechanically stable three-dimensional multilayer microchannels through a production process and a simple process. In this case, a three-dimensional microchannel or a three-dimensional multilayer structure may be formed by a single bonding process.

The film-type micro-reactor having a three-dimensional multi-layer microchannel manufactured by the present invention has a flexible feature, and can increase the yield by including a larger amount of microchannels than a conventional microreactor per unit thickness. In addition to being able to continuously react a series of reactions, it is possible to recycle the reaction to provide a variety of three-dimensional micro-reactor applications.

1 is a schematic diagram showing the lamination of one or more microchannels of the present invention by aligning the polymer film etched with metal pins.
2 is a schematic diagram showing a fine emulsifier having a three-dimensional coaxial flow according to Example 1 of the present invention.
Figure 3 shows the oil-in-water fine oil droplets according to Example 1 of the present invention by analyzing with an optical microscope.
4 is a schematic cross-sectional view of a three-dimensional membrane micromixer reactor according to Example 2 of the present invention.
Figure 5 shows a schematic diagram of the inside of the microchannel of the three-dimensional membrane (micrometer) micro mixer reactor according to the second embodiment of the present invention.
FIG. 6 shows a schematic diagram of a microemulsifier formed of a three-layer structure by stacking three microemulsifiers having a three-dimensional coaxial flow according to Example 3 of the present invention.
Figure 7 shows the oil-in-water fine oil droplets according to Example 3 of the present invention by analyzing with an optical microscope.

Hereinafter, the present invention will be described in more detail with reference to Examples.

At this time, the following examples are for the purpose of explanation, the present invention is not limited thereto.

Example 1

The microemulsifier having a three-dimensional coaxial flow was made by implementing the laminated structure of the polymer film according to the present invention. The fine emulsifier forms a microchannel 200 μm wide and 80 μm deep using a first layer film (Polyimide HN type, Dupont., USA) having a thickness of 125 μm using a laser, and a second layer film having a thickness of 25 μm ( PIXEO BP, KANEKA., JAPAN) was used to form microchannels of 25 μm width, 25 μm depth, 200 μm width, and 25 μm depth using a laser, and a 125 μm thick third layer film (Polyimide HN type, Dupont) , USA) using a laser to form a microchannel 200 μm wide, 80 μm deep, and then laminated each film to put a metal weight of more than 4 kg in the electric furnace and the film for 2 hours at a temperature of 320 ℃ The film was left to be bonded to each other and then cooled.

The prepared microemulsifier was connected to an aluminum chip holder (ICH-03, IMT, Japan), and the fluorocarbon oil or hexadecane or corn oil or edible oil was added to the fluid inlet formed in the first layer film at 1 to 5000 μl / min. Three-dimensional fine flow formed by stacking the first layer, the second layer, and the third layer by flowing distilled water into two different fluid inlets formed in the first layer film, flowing in the microchannel formed on the film of the second layer. It was allowed to flow in the channel, emulsifying the incoming oil while surrounding the incoming fluorocarbon oil or hexadecane or corn oil or edible oil to prepare oil-in-water microdroplets having a diameter of 10 to 100 ㎛. Thus prepared oil-in-water droplets could be confirmed using an optical microscope. (FIG. 2) (FIG. 3)

[Example 2]

In the method according to the present invention, a three-dimensional membrane micromixer reactor having a three-dimensional fluid flow and a membrane permeation flow by a plurality of micro holes is laminated by laminating a film having a plurality of micro holes in a micro reactor with a film having a micro channel. Produced. The micro-reactor forms a microchannel 800 μm wide and 80 μm deep using a laser on a 125 μm thick first layer film (Polyimide HN type, Dupont., USA), and a 25 μm thick second layer film ( PIXEO BP, KANEKA., JAPAN) using a laser to form a plurality of micro holes having a diameter of 25 ㎛ to be located in the channels formed in the film of the first and third layers, the third layer film having a thickness of 125 ㎛ (Polyimide HN type, Dupont., USA) using a laser to form a microchannel of 800 ㎛ width, 80 ㎛ depth, each film is laminated and put a metal weight of more than 4 kg in the electric furnace and 320 ℃ The film was allowed to stand for 2 hours at a temperature to be bonded to the film, and then cooled.

(FIG. 4) (FIG. 5)

[Example 3]

By stacking three microreactors prepared in Example 1 through the implementation of the laminated structure of the polymer film according to the present invention, a three-dimensional microchannel was formed in a microemulsifier. A fluid inlet and a fluid outlet were equally connected to each film to each of the polymer films etched in Example 1 to prepare a three-layer microemulsifier having one fluid inlet and a fluid outlet. The 3-layered microemulsifier was connected to an aluminum chip holder (ICH-03, IMT, Japan) to disperse the fluorocarbo oil or hexadecane in the microchannels formed in the first layer, the second layer, and the third layer structure. Corn oil or cooking oil was introduced at 1 to 5000 μl / min, and distilled water was introduced at 1 to 5000 μl / min in a continuous phase through the microchannels of the first, second and third layers. Fluorine carbon oil or hexadecane or corn oil or edible oil was prepared in bulk in a three-dimensional multi-layer microemulsifier having a three-layer structure. Thus prepared fine oil droplets could be confirmed by using an optical microscope (Fig. 6) (Fig. 7).

Claims (15)

(A) etching the polymer film to form one or more microchannels:
(b) laminating at least three polymer films on which at least one channel is formed by using metal pins, and further laminating a reinforcement film having a melting point lower than the temperature used for the bonding process at the top and the bottom thereof. ; And
(c) a method of manufacturing a film-type micro-reactor having three-dimensional multilayer microchannels comprising at least three laminated polymer films in a one-step multilayered bonding process. The method of claim 1,
The polymer film of step (a) is a film having a three-dimensional multi-layer micro-channel formed by etching the fluid input portion, the micro-channel portion through which the fluid flows, or the fluid discharge portion through which the introduced fluid is discharged using a laser Method for producing a type micro reactor. The method of claim 1,
The polymer film is polyimide, polyethylene, polyethylene, fluorinated ethylene propylene, polypropylene, polyethylene terephthalate, polyethylene naphthalate, or polysulfone Method for producing a film-type micro-reactor having a three-dimensional multilayer microchannel containing polysulfone). The method of claim 1,
The polymer film is a method of producing a film-type micro-reactor having a three-dimensional multilayer microchannel, characterized in that the homogeneous or heterogeneous film of 10 ~ 200 ㎛ thickness. The method of claim 1,
The method of manufacturing a film-type micro-reactor having a three-dimensional multilayer microchannels, characterized in that the microchannel of step (a) is a ratio of 1/5 to 1 of the polymer film thickness. The method of claim 1,
The lamination of step (b) is a method of manufacturing a film-type micro-reactor having a three-dimensional multi-layer micro-channel, characterized in that to form a hole in the same position on each corner of the polymer film in which the micro-channel is formed using a metal pin. The method of claim 1,
The single bonding process of step (c) is a film type micro-channel having a three-dimensional multilayer microchannel, characterized in that the laminated film is integrally bonded by heating and pressing at a temperature of the glass transition temperature (T _g ) to the melting point of the polymer film. Method for producing a reactor. delete The method of claim 1,
The method of manufacturing a film-type micro-reactor having a three-dimensional multilayer microchannel comprising further laminating a polymer film having a melting point higher than the temperature used in the bonding process between the reinforcement film and the polymer film etched microchannel. The method of claim 1,
Method for producing a film-type micro reactor having a three-dimensional multi-layer micro-channel having a total inlet rate of 1 ~ 5000 μl / min when one or more fluids are introduced. The method of claim 1,
Method for producing a film-type micro-reactor having a three-dimensional multilayer microchannel characterized in that a multi-layered multi-channel structure by performing a single bonding process of the three or more laminated polymer film. The method of claim 1,
The reactor is a method of producing a film-type micro-reactor having a three-dimensional multi-layered microchannel capable of carrying out one or more reactions by introducing one or more fluids. The method of claim 1,
The reactor is a method of producing a film-type micro-reactor having a three-dimensional multilayer microchannel capable of continuously reacting a series of reactions. The method of claim 1,
The reactor is a method of producing a film-type micro-reactor having a three-dimensional multilayer microchannel capable of recycling reaction. The method of claim 1,
The reactor is a method of producing a film-type micro reactor having a three-dimensional multilayer microchannel, characterized in that it has flexibility.

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