JP5504526B2 - Method of forming slag flow using a microreactor - Google Patents

Description

This invention relates to a microreactor for implementing the mixing and reaction of the microfluidic required microchemical process, in particular a micro reactor (active to actively utilize the change in the appearance of the slag to achieve a reactor features high efficiency Slag reactor) .
The present invention is closely related to organic synthetic chemistry, analytical chemistry, chemical engineering, mechanical engineering, biochemistry, and the like, and can be immediately applied to various industrial chemical processes.

“Mixing” is an important function required for devices for microchemical processes, and examples of known mixing apparatuses for microchemical processes have been proposed or have already been used.
(1) A mixing method using mechanical stirring (for example, a micro mixer manufactured by IMM, Germany).
(2) A mixing method using alternating flow (for example, see Non-Patent Document 1).
(3) A mixing method using a T-junction (for example, see Non-Patent Document 2).
(4) A mixing method using a Y-junction (for example, see Non-Patent Document 3).
Donata et al., Chem. Eng. J. 135S (2008) S37-S45. Soleymani et al., Chem. Eng. J. 135S (2008) S219-S228. Batoul et al., Chem. Eng. J. 135S (2008) S280-S283.

  However, the methods (1) and (2) are both large in size and complicated in structure, so that their size, weight and price are not suitable for microchemical processes. For example, the liquid-liquid micromixer of IMM in Germany is composed of simple patterns of flow paths and connects them, but it includes unnecessary parts (such as joint parts) other than the mixing site, so the device is The size of the microreactor is one of the causes that make it difficult to reduce the size of the microreactor.

  The above methods (3) and (4) are simple and general methods for solving the disadvantages of the methods (1) and (2). Road) and Y-pipe (Y-junction) have been proposed as "a method of using turbulence generated when a fluid collides" and "a method of using a collision turbulent flow caused by a discharge jet flow". The method has the greatest drawback in that the occurrence of disturbance is only one place, and in particular, the continuity of disturbance cannot be realized.

  Therefore, the present inventors have applied for a patent considering a method of increasing the number of collisions as one of the methods for continuously generating disturbance. However, as a method of continuously maintaining turbulence by increasing the number of collisions, the method of repeating merging and separation is used, resulting in a longer flow path length and more complicated processing of the flow path. There are some points to be improved, such as high costs.

  And in these pipe and tube connection methods and jet flow collision methods, the flow conditions such as the flow characteristics of the target fluid are accurately set in addition to the dimensional conditions such as the posture, positional relationship, and length of the flow path. It is very difficult to maintain the certainty and continuity of the turbulent state, which may cause instability in the flow characteristics and cause variations in the mixing characteristics.

  Therefore, the present invention has a structure for enabling the miniaturization and integration of the microreactor by actively utilizing the change in the appearance of the slag generated by a plurality of fluids to be mixed inside the microchannel for the mixing and reaction. The purpose is to propose.

  In order to advantageously solve the above problems, the present invention proposes a device for a microchemical process having a concavo-convex channel inner surface structure for expressing a deforming slag with respect to a slag flow by two or more fluids. The simple and original flow channel structure provides a highly efficient mixing function that enables continuous disturbance. More specifically, the flow channel width is several tens of μm to several mm. As an effective measure to obtain high-efficiency mixing by generating turbulence reliably and continuously in the fluid flowing in the slag flow, the effect of symmetrical irregularities on the inner surface of the flow path (straight, polygonal) In addition, the present invention proposes a structure in which the unevenness due to the arc or the like is symmetrical with respect to the axis), the asymmetric unevenness effect on the inner surface of the flow path, the cross-sectional area change effect due to the shape of the inner surface of the flow path, or the like.

That is, the method of forming a slug flow using microreactor of the present invention, a micro that Ru comprising a flow path connecting between the confluence point and the outlet with connecting inlet channel leading to each of the plurality of inlets at confluence using reactor, the fluid in the flow channel compatibility plurality of types without fluid was allowed to flow from the plurality of inlets, each a method of forming a slug flow appearing alternately, the meeting point and the outlet The inner surfaces facing each other of the flow path connecting between and each of the flow paths are formed by repeatedly arranging concave and convex portions that are concave and convex with respect to the flow path along the flow path. The minimum distance between the convex portions facing each other is the distance that allows the slag of the slag flow flowing in the flow path to move to the outlet while simultaneously contacting both opposing convex portions, Said each other Interior surface direction is, is characterized in that the slag is to guide along the flow path while deformed along a said recess and protrusion.

In the present invention comprising such a structure, mutually opposing inner surfaces of the flow path connecting between the confluence and outlet have respective uneven aligned along the flow path, between the inner surfaces facing each other Since the minimum distance is the distance that the slag of the slag flow flowing in the flow path can move while simultaneously contacting both of the inner surfaces facing each other, the slag of the slag flow flowing in the flow path from the inlet to the outlet is It moves while touching both of the inner surfaces facing each other at the same time (but not necessarily to the depth of the recesses on the inner surface), and the unevenness of these inner surfaces generally adds slag to the unevenness. Therefore, the turbulence is reliably and continuously generated in the slag and in the fluid in the vicinity of the slag during the movement of the slag in the flow path while being deformed.

Therefore, according to the present invention , it is possible to efficiently generate mixing / reaction of fluid in the slag, extraction / mixing / reaction via the interface between the slag and the fluid in the vicinity thereof, and the like. It solves the problem of the complicated flow channel structure and creation process, which makes it possible to shorten the flow channel length and easily create the microreactor and to reduce the size and integration of the microreactor. And parallel processing can be easily realized.

Note that the configuration Oite to the present invention, the flow path is a slit formed in the plate sandwiched between two members or by being formed on the surface of the member or plate which is covered with another member groove The inner surfaces facing each other may be the wall surfaces of the slits or the grooves. In this way, when the plate is sufficiently thin, the slits form a micro flow path, and are formed on the surface of the member or the plate. If the depth and width of the formed groove are sufficiently small, a microchannel with a width and depth of several tens of μm to several mm is formed, so that the microreactor can be easily downsized and integrated. Can do.

Further, Oite to the present invention, the minimum distance between the inner surfaces of said opposite each other, the may be larger the greater the contact angle of the inner surface and the slag, in this manner, for example, under the trade name Teflon ( By forming the flow path inner surface with a material having a large contact angle with a slag such as a trademark, the minimum distance between the inner surfaces facing each other can be increased to increase the flow rate.

Furthermore, Oite to the present invention, concave and convex portions of the inner surface of the facing each other may have a symmetrical cross-sectional shape relates axis of the channel, along the easy passage Thus Since the cross-sectional area of the flow path can be changed, the slag can be more reliably deformed.

On the other hand, Oite to the present invention, concave and convex portions of the inner surface of the facing each other, may have an asymmetrical sectional shape relates axis of the channel, the deformation of the slug so doing also asymmetrically Therefore, more mixing and reaction of the fluid in the slag can be caused.

Furthermore, Oite to the present invention, the sectional shape of the concave and convex portions of the inner surface of the facing each other, the channel saw blade shape and a bent portion linear portion extending obliquely relative to the axis are alternately repeated in In this way, the slag can be smoothly deformed to reduce the channel resistance.

On the other hand, Oite to the present invention, the sectional shape of the concave and convex portions of the inner surface of the opposing, which may be a shape which is a combination of arcs, in this manner, to rapidly deform the slag slag It is possible to generate more mixing and reaction of the fluid inside.

Furthermore, Oite to the present invention, the sectional shape of the concave and convex portions of the inner surface of the opposing, which may be a shape of a combination of a circular arc and a straight line, while reducing the flow resistance in that case Many mixing and reaction of the fluid in the slag can occur.

Furthermore, Oite to the present invention, the flow path may not extend spirally, in this manner, be obtained by forming a long flow path by Kagire was wide in the region, the microreactor It is possible to more easily reduce the size and the integration.

Then, Oite to the present invention, the flow path, be combined in parallel a plurality, also may be combined in several series, in this manner, miniaturization of the microreactor, integration It can be made easier.

Hereinafter, embodiments of the present invention will be described in detail with reference to the drawings. Here, FIGS. 1A, 1B, 1C, and 1D are a plan view, a side view, and a flow channel detail showing an embodiment of a microreactor (also referred to as an active slag reactor) according to the present invention. FIG. 1 is a detailed view of the part A, in which 1 is the microreactor of this embodiment, 2 is the first inlet, 3 is the second inlet, 4 is the outlet, and 5 is the inlets 2, 3 and the outlet 4 are respectively shown. In addition, the dimension in each following Example is an illustration to the last, and the microreactor regarding this invention is not limited to the thing of these dimensions.

In the embodiment shown in FIG. 1, a slit 6 having a width of 0.5 mm to 1.3 mm penetrating vertically is formed in a plate 6 made of stainless steel (SUS 304) having a thickness t of 0.3 mm. , 3 and constitutes a micro reactor 1 comprising a flow path 5 connecting the outlet 4, the flow path 5 from the inlet 2, 3 merge at the merging point I, the flow from the joining point I to the outlet 4 The path 5 has inner surfaces 5a and 5b facing each other formed by the wall surfaces of the slits, and the cross-sectional shape of the inner surfaces 5a and 5b cut along a plane parallel to the surface of the plate 6 is shown in FIG. ), A sawtooth shape symmetrical with respect to the central axis C of the flow path 5 (a shape in which linear portions and bending portions extending obliquely with respect to the central axis C of the flow path 5 are alternately repeated) is formed. Yes.

  More specifically, the cross-sectional shapes of the inner surfaces 5a and 5b facing each other are more specifically two reference lines that are symmetrical with respect to the central axis C and intersect the central axis C at an angle of 30 ° and are separated from each other by a maximum of 1 mm. 5c is defined to extend parallel to the reference line 5c with a distance of 0.15 mm on the outer side, and in this embodiment, each of the saw-tooth-like irregularities on the inner surfaces 5a and 5b is defined. The angle formed by the tip is 120 °, the minimum distance between the inner surfaces 5a and 5b is about 0.35 mm, and the maximum distance is about 1.35 mm. The angle formed by the tips of the sawtooth irregularities may be 90 ° as shown in the modified example of FIG. 1 (e), but 120 ° is the surface tension of the slag within the concave shape. This is preferable because the slag comes into contact with the back of the concave shape and is sufficiently deformed.

  The plate 6 is made of, for example, quartz glass, which is approximately the same size, made of quartz glass, for example, when it is possible to observe a slag flow, and made of stainless steel, for example, for reaction purposes only. Two inlet channels that are tightly sandwiched by the thick plates, distributed to one or both of the thick plates and connected to the first inlet 2 and the second inlet 3, respectively, and the outlet 4 A connected outlet channel is formed. As a result, fluids alternately flowing from the two inlet channels into the first inlet 2 and the second inlet 3 merge at the junction I to form a slag flow (so-called each fluid flows alternately). Then, the plug flow flows from the confluence point I toward the outlet 4 in the flow path 5 and then flows out from the outlet flow path through the outlet 4.

Figure 2 is an explanatory view showing the results of an experiment to flow plug flow micro reactor 1 of the flow path of this embodiment, the plate 6 and sandwiched between two thick plates made of quartz glass, blue When water A of the water is alternately introduced from the first inlet 2 and orange cyclohexane B is alternately introduced from the second inlet 3 to form a slag flow at the junction, a slag (fluid element: code) of the slag flow is formed. The same slag as the fluid is used.) Of A and B, the water slag A rounded by its own surface tension is pushed by the saw-toothed irregularities of the inner surfaces 5a and 5b to form a shape like a cloud. It is deformed and moves toward the outlet 4 while continuously moving the constricted part to the rear of the flow.

Therefore, according to the micro reactor 1 of this embodiment, two types of liquid or liquid and gas or mixed-reactions and in the slag in the plug flow consisting of liquid and powder, etc., slag and the vicinity thereof of the fluid Extraction, mixing, reaction, etc. can be efficiently generated through the interface between them, and since the flow path structure and creation process are both simple, the flow path length can be shortened and created easily. Therefore, the microreactor can be miniaturized and integrated.

3 (a), (b), (c), and (d) are a plan view, a side view, a flow path detail view, and a part A detail view showing another embodiment of the microreactor according to the present invention. In the figure, the same parts as those in the previous embodiment are denoted by the same reference numerals. In the microreactor 1 of this example, the cross-sectional shape of the inner surfaces 5a and 5b facing each other of the flow path 5 cut by a plane parallel to the surface of the plate 6 is as shown in FIG. This embodiment differs from the previous embodiment only in that it is composed of a number of substantially semicircular shapes arranged along the flow path 5 so as to be symmetric with respect to the central axis C. It is configured.

  More specifically, the cross-sectional shape of the inner surfaces 5a and 5b facing each other is more specifically set to the outer side of the two reference lines 5c extending parallel to the central axis C and spaced apart from each other by 0.3 mm. A large number of circular arcs with a radius of 0.15 mm centered on the upper point are drawn symmetrically with respect to the central axis C at a pitch of 0.355 mm, and these arcs are connected by an arc with a radius of 0.03 mm. In the embodiment, the minimum distance between the inner surfaces 5a and 5b is 0.3 mm, and the maximum distance is about 0.6 mm.

According to the micro reactor 1 of this embodiment, in addition to being able to bring about the same effect as the previous embodiment, in particular, the inner surface 5a, the convex shape of 5b can significantly deformation degree of steep because slag In addition, mixing / reaction in the slag, extraction / mixing / reaction, etc. via the interface between the slag and the fluid in the vicinity thereof can be generated more efficiently.

FIGS. 4A, 4B, and 4C are a plan view, a side view, and a flow channel detail diagram showing another embodiment of the microreactor according to the present invention, in which the same as the previous embodiment. This part is indicated by the same reference numeral. In the microreactor 1 of this embodiment, the cross-sectional shape of the inner surfaces 5a and 5b facing each other of the flow path 5 cut by a plane parallel to the surface of the plate 6 is as shown in FIG. 1 is different from the embodiment shown in FIGS. 1 and 3 only in that it is made up of a number of substantially semicircular shapes arranged along the flow path 5 so as to be asymmetric with respect to the central axis C of the above. The configuration is the same as that of the embodiment.

  More specifically, the cross-sectional shape of the inner surfaces 5a and 5b facing each other is more specifically defined by the inner surface 5a and the inner surface 5b with respect to two reference lines 5c extending in parallel to the central axis C and spaced apart from each other by 0.3 mm. Then, a large number of arcs with a radius of 0.15 mm centering on a point located symmetrically with respect to the central axis C on the reference line 5c are drawn side by side, and these arcs are connected by arcs of the smallest radius that can be processed. Thus, in this embodiment, the shape of the inner surface 5a is translated by 0.3 mm in the direction perpendicular to the central axis C to obtain the shape of the inner surface 5b, and the minimum distance between the inner surfaces 5a and 5b is set. It is smaller than 0.3 mm between the convex part of the inner surface 5a and the convex part of the inner surface 5b.

According to the micro reactor 1 of this embodiment, in addition to being able to bring about the same effect as the previous embodiment, in particular, because the inner surface 5a, uneven shape 5b forms an asymmetric with respect to the central axis C Since the deformation of the slag can be made asymmetric with respect to the central axis C, the mixing / reaction in the slag and the extraction / mixing / reaction via the interface between the slag and the fluid in the vicinity can be generated more efficiently. Can do.

FIGS. 5A, 5B, and 5C are a plan view, a side view, and a flow channel detail diagram showing still another embodiment of the microreactor according to the present invention. Similar parts are denoted by the same reference numerals. In the microreactor 1 of this example, the cross-sectional shape of the inner surfaces 5a and 5b facing each other of the flow channel 5 cut by a plane parallel to the surface of the plate 6 is as shown in FIG. 1 is different from the embodiment shown in FIGS. 1 and 3 only in that it is made up of a number of substantially semicircular shapes arranged along the flow path 5 so as to be asymmetric with respect to the central axis C of the above. The configuration is the same as that of the embodiment.

  More specifically, the cross-sectional shapes of the inner surfaces 5a and 5b facing each other are more specifically defined by the inner surface 5a on the outer side and the inner side with respect to two reference lines 5c that extend parallel to the central axis C and are separated from each other by 0.3 mm. In order, on the inner surface 5b, a large number of arcs with a radius of 0.15mm centering on a point located symmetrically with respect to the central axis C on the reference line 5c are arranged side by side, and the arcs are connected to each other. Thus, in this embodiment, the shape of the inner surface 5a obtained by translating 0.3 mm in the direction perpendicular to the central axis C is the shape of the inner surface 5b, and the minimum distance between the inner surfaces 5a and 5b is the inner surface 5a. Between the convex portion of the inner surface 5b and the convex portion of the inner surface 5b.

According to the micro reactor 1 of this embodiment, in addition to being able to bring about the same effects as the embodiment shown in FIGS. 1 and 3, in particular, similarly to the embodiment shown in FIG. 4, the inner surface 5a, 5b of the Since the concavo-convex shape is asymmetric with respect to the central axis C, the deformation of the slag can be asymmetric with respect to the central axis C. Therefore, the mixing / reaction in the slag and the interface between the slag and the fluid in the vicinity thereof can be performed. Extraction, mixing, reaction, etc. can be generated more efficiently.

FIG 6 (a), (b) , (c) is a schematic diagram showing the inner surface 5a of the channel 5, 5b of the cross-sectional shape, respectively, in still another embodiment of the microreactor for this invention. FIG. 6 ( In the embodiment shown in a), the shape connecting the circular arcs is formed symmetrically with respect to the central axis on the inner surfaces 5a and 5b, and then one of the inner surfaces 5a and 5b is shifted by a half pitch, and the embodiment shown in FIG. In the example, after the shape connecting the arcs is formed on the inner surface 5a, the inner surface 5b is formed asymmetrically with respect to the inner surface 5a with respect to the center axis C by parallel translation in a direction orthogonal to the central axis. In the embodiment shown in FIG. 2, the inner surfaces 5a and 5b are formed symmetrically with respect to the central axis by connecting the arcs with straight lines. Also according to these embodiments, the same effects as those of the previous embodiments can be brought about.

Figure 7 is a schematic diagram showing a shape of the flow path 5 in still another embodiment of the microreactor for this invention, in this example, it is curved passage 5 extended by, in particular illustrated example spiral The cross-sectional shape of the inner surfaces 5a and 5b is a saw blade similar to the embodiment shown in FIG. The shape of the curve is not limited to a spiral shape as shown in the drawing, but may be a bellows shape, or a combination thereof.

According to the micro reactor 1 of this embodiment, in addition to being able to bring about the same effect as the previous embodiment, in particular, it is obtained by forming a long flow path 5 by the area of the breadth which is Kagire In addition, the microreactor can be more easily downsized and integrated.

FIG. 8 is a schematic diagram showing the configuration of the flow channel 5 in still another embodiment of the microreactor according to the present invention. In this embodiment, a plurality of rows of flow channels 5 having a saw blade-like inner surface (see FIG. combination three rows) parallel with示例constitutes their flow path microreactor by merging the outlet ends of 5, microreactor for this invention, the same or different types of the plurality of flow as in this embodiment In addition to combining the paths in parallel, a plurality of flow paths of the same or different types may be combined in series, or may be combined in parallel and in series. In this way, the microreactor can be more easily downsized and integrated.

Although the present invention has been described based on the illustrated example, the present invention is not limited to the above-described example, and can be appropriately changed within the scope of the claims. For example, the plate 6 is replaced with the product name Teflon ( (Registered trademark) or other material having poor wettability, or the wall surface of the slit forming the flow path 5 of the metal plate 6 such as stainless steel is covered with the material having poor wettability to form the inner surface. If the wettability of the inner surface of the flow path is deteriorated in this way, the two types of fluids in the flow path can be made difficult to become parallel flows even if the minimum distance between the inner surfaces of the flow path is increased. Thus, the flow resistance of the flow path can be further reduced. In the above example, the flow path is configured by the slit, but the flow path may be configured by a groove formed on the surface of the member.

Furthermore, in the above embodiment, the shape of the inner surface corresponding to the wall surface of the flow path is changed two-dimensionally. However, the shape of the inner surface corresponding to the upper and lower surfaces of the flow path may be changed two-dimensionally, or the flow The entire circumference (up / down / left / right) of the road may be three-dimensionally uneven.
Further, each of the embodiments other than FIGS. 6 and 8 has two inlets 2 and 3. However, if a slag flow is separately formed, a flow path as in each embodiment shown in FIGS. There may be only one entrance.

Thus , according to the present invention , the mixing / reaction of the fluid in the slag, the extraction / mixing / reaction via the interface between the slag and the fluid in the vicinity thereof can be efficiently generated, and the flow path The length of the microreactor can be easily reduced, the microreactor can be miniaturized and integrated, and parallel processing can be easily realized.

(A), (b), (c), (d) is the top view which shows one Example of the microreactor regarding this invention, a side view, a flow-path detailed view, and the A section detailed view. It is explanatory drawing which shows the result of having conducted the experiment which sends a plug flow in the flow path of the micro reactor 1 of the said Example. (A), (b), (c), (d) is a plan view, a side view, a flow path detail view, and a part A detail view showing another embodiment of the microreactor according to the present invention. (A), (b), (c) is the top view, side view, and flow-path detail figure which show another Example of the microreactor regarding this invention. (A), (b), (c) is the top view, side view, and flow path detail figure which show further another Example of the microreactor regarding this invention. (A), (b), (c) is a basic diagram which each shows the cross-sectional shape of the inner surface of the flow path in the further another Example of the microreactor regarding this invention. It is a basic diagram which shows the shape of the flow path in further another Example of the microreactor regarding this invention. It is a basic diagram which shows the structure of the flow path in another one Example of the microreactor regarding this invention.

1 micro reactor 2 first inlet 3 second inlet 4 outlet 5 passage 5a, cyclohexane C central axis I confluence 5b inner surface 5c reference line 6 plates A blue water B orange

Claims (11)

Using a microreactor Ru comprising a flow path connecting between the confluence point and the outlet with connecting inlet channel leading to each of the plurality of inlets at the merging point, the plurality of compatibility without a plurality of types of fluids, respectively A method of forming a slag flow in which each fluid appears alternately in the flow path by flowing from an inlet,
The inner surfaces facing each other of the flow path connecting the junction and the outlet are each formed by repeatedly arranging concave and convex portions that are concave and convex with respect to the flow path along the flow path. ,
The minimum distance between the convex portions facing each other across the flow channel is a distance that allows the slag of the slag flow flowing in the flow channel to move to the outlet while simultaneously contacting both the convex portions facing each other. Yes,
A method of forming a slag flow using a microreactor, wherein the inner surfaces facing each other guide the slag along the flow path while deforming the slag along the concave and convex portions. The flow path is constituted by a slit formed in a plate sandwiched between two members or a groove formed on the surface of a member or plate and covered with another member,
The method for forming a slag flow using a microreactor according to claim 1, wherein the inner surfaces facing each other are wall surfaces of the slits or the grooves. 3. The method of forming a slag flow using a microreactor according to claim 1, wherein a minimum distance between the inner surfaces facing each other is increased as a contact angle between the inner surface and the slag is increased. . The slag flow using the microreactor according to any one of claims 1 to 3, wherein the concave portions and the convex portions of the inner surfaces facing each other have a symmetric cross-sectional shape with respect to the axis of the flow path. How to form . The slag flow using the microreactor according to any one of claims 1 to 3, wherein the concave portions and the convex portions of the inner surfaces facing each other have a cross-sectional shape that is asymmetric with respect to an axis of the flow path. How to form . The cross-sectional shapes of the concave portions and the convex portions on the inner surfaces facing each other have a saw-tooth shape in which linear portions and bent portions extending obliquely with respect to the axis of the flow path are alternately repeated. A method for forming a slag flow using the microreactor according to any one of claims 1 to 5. 6. The slag flow using the microreactor according to claim 1, wherein the cross-sectional shapes of the concave portion and the convex portion on the inner surfaces facing each other are a combination of circular arcs. How to form . The microreactor according to any one of claims 1 to 5, wherein the cross-sectional shapes of the concave portion and the convex portion of the inner surfaces facing each other are a combination of a circular arc and a straight line. To form a slug flow . The method for forming a slag flow using the microreactor according to any one of claims 1 to 8, wherein the flow path extends in a spiral shape. The method for forming a slag flow using the microreactor according to any one of claims 1 to 9, wherein a plurality of the flow paths are combined in parallel. The method for forming a slag flow using the microreactor according to any one of claims 1 to 10, wherein a plurality of the flow paths are combined in series.

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