JP2009241031A - Reactor and reaction apparatus using it - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a reactor capable of improving the reaction of a raw material and of being operated by low power consumption. <P>SOLUTION: A heating resistor 5c is provided to an introducing pipe 5a and lead-out pipe 5b inserted through a substrate 1 and joined to the substrate 1 through a solder material 3. When joining the introducing pipe 5a and the lead-out pipe 5b, it is made possible to apply heat locally and the scattering or the like of impurities from the substrate 1 is suppressed to prevent not only the thermal breakage of parts provided to the reactor 10 but also the adhesion of scattered matter to internal parts caused by the scattering or the like of impurities from the substrate 1 even when the heat resistance of the parts provided to the reactor 10 is low. <P>COPYRIGHT: (C)2010,JPO&INPIT

Description

  The present invention relates to a reactor and a reaction apparatus using the reactor.

  In recent years, a microreactor focused on the point that it shows a chemical reaction different from that during mass processing by charging the raw material into the reactor and heating or kneading the raw material flowing through the fine space formed inside The technology about is attracting attention. For example, since the two liquid raw materials are kneaded, the reaction continues to occur at the portion where the two liquids flowing through the fine flow path come into contact with each other, so that very efficient processing is possible.

  Furthermore, recently, not only pipes for inputting / outputting raw materials but also introduction pipe and outlet pipe structures capable of inputting / outputting raw materials accurately and with high strength have been studied.

  In addition to having a flow path through which the raw material circulates, an electrode for energizing a heating means for heating the raw material is also provided, and a reactor in which several functions are integrated has been proposed. ing.

JP 2003-2602 A

  In the process of manufacturing the reactor, with respect to the introduction pipe and the lead-out pipe for inputting and outputting the raw materials, the reactor main body, the introduction pipe and the lead-out pipe are brazed by a method of heating the entire reactor.

  If the heat resistance of the parts provided in the reactor is low, the parts may be destroyed, or impurities may scatter from the substrate, resulting in problems such as failure to obtain a correct reaction of the raw materials or contamination of the raw materials. there were.

  Therefore, there has been a demand for a reactor that improves the reaction of raw materials and a reaction apparatus using the reactor.

  A reactor according to an embodiment of the present invention includes a base body having an internal space, a dielectric, an introduction pipe and a lead-out pipe that are inserted through the base body and joined to each other via a brazing material, Heating means provided in the introduction pipe and the outlet pipe.

  According to the reactor according to the embodiment of the present invention, the heating means is provided in the introduction pipe and the outlet pipe that communicate with the inside and outside of the base body and are joined to the base body via the brazing material. Even if the whole is not heated, heating by local heating is possible.

  Therefore, even if the heat resistance of the components provided in the reactor is low, the components may be destroyed by heat, or scattered matter may adhere to the internal components due to scattering of impurities from the substrate. Since it can suppress, a stable chemical reaction can be produced. In addition, before and after the reaction of the raw material, depending on the raw material, when the characteristics such as the presence or absence of corrosion of the brazing material connecting the introduction pipe and the discharge pipe to the base body are different, for the introduction pipe to which the raw material before the reaction is supplied Thus, it is possible to selectively use brazing materials having different characteristics, such as a brazing material for an exhaust pipe from which the raw material after reaction is discharged. As a result, a highly reliable reactor can be constructed.

  FIG. 1 is a cross-sectional view of a reaction apparatus 12 including a reactor 11 showing an embodiment of the present invention, and FIG. 2 is a cross-sectional view of the reactor 11 shown in FIG.

  The reactor 11 of the present embodiment includes a brazing material 3, an introduction pipe 5a that is a supply path for supplying raw materials, a discharge pipe 5b that is a discharge path for discharging raw materials after reaction, a heating resistor layer 5c, an electrode 7 and A substrate (reactor body) 10 is provided.

  In addition, the reaction apparatus 12 of the present embodiment includes the above-described reactor 11, a rectangular plate-like substrate 1, and a casing 9 including a rectangular parallelepiped box-like lid 4. In this case, the lid 4 is mounted on the substrate 1, and the supply pipe 5a and the discharge pipe 5b are connected to the substrate 1, whereby the reaction apparatus 12 is configured.

  In the present invention, the supply pipe 5a and the discharge pipe 5b are not limited to those connected to the substrate 1, but may be connected to the lid 4 side.

  Hereinafter, each component is demonstrated about the reactor 11 and the reaction apparatus 12 which concern on one Embodiment of this invention.

(Reactor body)
The reactor 11 according to the present embodiment has a reaction path including a groove, a gap, and the like for allowing the raw material to flow inside the substrate (reactor body) 10. Various shapes can be adopted as the shape of the substrate (reactor body) 10.

  For example, the substrate (reactor body) 10 can be manufactured as a microchemical device. The substrate (reactor body) 10 is manufactured by first applying a semiconductor manufacturing technology or the like to a semiconductor such as silicon, an inorganic material such as quartz, glass or ceramics, or a base material such as a metal. A thin groove is formed by an etching method, a blast method, or the like, and a reaction path for reacting the raw material is prepared. Next, for the purpose of preventing evaporation of the liquid flowing through the reaction path, a glass plate, a metal cover, etc. is bonded to the substrate so as to cover the reaction path by anodic bonding, brazing, welding or the like. Further, like the ceramic laminated structure, the cover may not be joined later, and the reaction path and the portion to be the cover may be integrated. As described above, the substrate (reactor body) 10 can be produced.

  The substrate (reactor body) 10 is formed in a hollow and rectangular parallelepiped shape, for example. Further, the material of the substrate (reactor body) 10 may be made of an inorganic material such as quartz, glass or ceramics, or a metal, and includes an inner surface on which a catalyst for reacting the raw material is supported.

  The reactor 11 according to the embodiment of the present invention heats a raw material to cause a chemical reaction on the surface of the substrate (reactor body) 10 or inside the substrate (reactor body) 10. Thin film heaters and thick film heaters composed of body layers are formed. For example, as shown in FIGS. 1 and 2, an electrode 7 is formed as a terminal on the surface of the substrate (reactor body) 10, and the electrode 7 is connected to the bonding wire 3 or the like. By being electrically connected to the lead terminal 8 through the conductive bonding material, electric power is supplied from the outside. In FIG. 1, the lead terminal 8 also serves as the heating resistor layer 5c.

  By adjusting the temperature corresponding to the raw material reaction conditions by this temperature adjusting mechanism, for example, a temperature condition of about 20 ° C. to 800 ° C., the raw material supplied from the raw material supply port connected to the introduction pipe 5a is reacted, The chemical reaction for generating the liquid or gas after the reaction from the outlet pipe 5b connected to the discharge port can be favorably promoted.

  Moreover, as a heating resistor layer, a thing with high electrical resistance is preferable, for example, Mo-Mn, W, Pt, etc. are used. With respect to such a heating resistor layer, the surface of the substrate (reactor main body) 10 only needs to be an insulator or a semiconductor at least in a portion that is in electrical contact with the heating resistor layer. Therefore, as the substrate (reactor body) 10, the entire substrate (reactor body) 10 may be made of an insulator or a semiconductor, or only a part may be made of an insulator or a semiconductor. .

(Introducing pipe and outlet pipe)
The introduction pipe 5a and the lead-out pipe 5b can use various dielectric materials.

When the introduction pipe 5a and the lead-out pipe 5b are made of glass ceramics, they are made of a glass component and a filler component. Examples of the glass component include SiO ₂ —B ₂ O ₃ system, SiO ₂ —B ₂ O ₃ —Al ₂ O ₃ system, SiO ₂ —B ₂ O ₃ —Al ₂ O ₃ —MO system (where M is Ca, Sr, Mg, Ba or Zn), SiO ₂ —Al ₂ O ₃ —M ¹ O—M ² O system (where M ¹ and M ² are the same or different, Ca, Sr, Mg, Ba or Zn represents), SiO ₂ —B ₂ O ₃ —Al ₂ O ₃ —M ¹ O—M ² O system (where M ¹ and M ² represent the same or different Ca, Sr, Mg, Ba or Zn) ), SiO ₂ —B ₂ O ₃ —M ³ ₂ O system (where M ³ represents Li, Na or K), SiO ₂ —B ₂ O ₃ —Al ₂ O ₃ —M ³ ₂ O system ( M ³ represents Li, Na or K), Pb glass, Or Bi glass etc. are mentioned.

Examples of the filler component include Al ₂ O ₃ , SiO ₂ , a composite oxide of ZrO ₂ and an alkaline earth metal oxide, a composite oxide of TiO ₂ and an alkaline earth metal oxide, or Al _2. Examples thereof include composite oxides containing at least one selected from O ₃ and SiO ₂ (for example, spinel, mullite, cordierite) and the like.

  On the other hand, when the introduction pipe 5a and the lead-out pipe 5b are formed of a dense aluminum oxide sintered body having a relative density of 95% or more, for example, first, rare earth oxide powder or aluminum oxide is added to the aluminum oxide powder. A sintering aid such as powder is added and mixed to prepare a raw material powder of the aluminum oxide sintered body. Next, an organic binder and a dispersion medium are added to this raw material powder, mixed to form a paste, and this paste is introduced by a doctor blade method, or an organic binder is added to the raw material powder, and a predetermined shape is introduced by press molding, rolling molding, etc. After forming the pipe 5a and the lead-out pipe 5b, for example, firing in a non-oxidizing atmosphere at a firing maximum temperature of 1200 ° C. to 1500 ° C. to obtain the target ceramic lead-in pipe 5a and lead-out pipe 5b Can do. The introduction tube 5a and the lead-out tube 5b may be formed by a powder forming press method or a laminate formed by laminating green sheets.

  Further, when the introduction pipe 5a and the lead-out pipe 5b are made of a metal material, it is preferable to form an oxide film or the like on the surface to make it a dielectric. For example, an oxide film may be chemically formed on the surface of Al by an electrochemical method using Al as an anode, or by artificially growing an oxide film or using an acidic or alkaline aqueous solution.

(Heating means)
Hereinafter, the case where the heating resistor layer 5c is provided as an example of the heating means will be described.

  The heating resistor layer 5c is provided in close contact with each outer peripheral surface of the introduction pipe 5a and the outlet pipe 5b in the reactor 11. As a result, the reactor 11 according to the present embodiment can not only apply heat locally when the pipe is joined, but also when the entire reactor is not heated, and has the following effects.

  Further, the reactor 11 heats the introduction pipe 5a and the lead-out pipe 5b when the raw material is circulated through the introduction pipe 5a or when the product after the raw material reaction is circulated through the lead-out pipe 5b. The heat generated from each heating resistor layer 5c, such as preheating or afterheating that causes heat generation, can be efficiently used for the reaction of the raw material.

  Further, by providing the heating resistor layer 5c on the introduction pipe 5a and the lead-out pipe 5b, respectively, the cross-sectional rigidity of the part where the heating resistor layer 5c of the lead-in pipe 5a and the lead-out pipe 5b is provided is improved. The pipe 5a and the outlet pipe 5b are reinforced. The thickness of the heating resistor layer 5c is preferably 0.5 μm to 500 μm from the viewpoint of efficiently supplying heat to the reaction path and from the viewpoint of improving the strength.

  Such a heating resistor layer 5c may be provided in the walls of the introduction pipe 5a and the lead-out pipe 5b. As a result, the raw material such as gas can be directly heated, so that the raw material can be easily introduced into the reactor 11 in a state where it can be activated. The thickness of the heating resistor layer 5c is preferably 0.5 μm to 500 μm from the viewpoint of efficiently supplying heat to the reaction path and the smooth supply / discharge of the raw material. In consideration of the case of supplying and discharging the liquid, it is preferable to form an electrical insulator layer on the surface so as to be electrically insulated from the introduction pipe 5a and the lead-out pipe 5b.

  Further, such a heating resistor layer 5c is provided between the layers forming the introduction pipe 5a and the lead-out pipe 5b, and the respective layers may be connected by vias or the like as necessary. As a result, since the heating resistor is not directly in contact with a raw material such as gas, it is less susceptible to corrosion, so the heating resistor is not corroded and has no problems such as opening. Since stable heat generation is always possible, the raw material can be introduced into the reactor 11 in a state where it can be easily activated. The thickness of the heating resistor layer 5c is preferably 0.5 μm to 500 μm from the viewpoint of efficiently supplying heat to the reaction path and the smooth supply / discharge of raw materials. In addition, considering the case of supplying and discharging conductive raw materials, it is not necessary to form an electrical insulator layer on the surface and electrically insulate from the introduction pipe 5a and the lead-out pipe 5b. Since it becomes possible to make it react, it can be set as a more versatile reactor.

  Further, the heat generating resistor layer 5c may be formed by metallizing a non-metallic body such as glass or ceramic, and adherence to the introduction pipe 5a and the outlet pipe 5b made of a non-metallic body such as glass or ceramic. The raw material flowing through the introduction pipe 5a and the lead-out pipe 5b can be heated more efficiently, and the reactor 11 with high responsiveness in heating temperature control can be realized.

Inlet tube 5a and outlet tubes 5b heating resistor layer 5c is provided in, for example, _Al 2 _{O 3} sintered _material, 3Al ₂ O 3 · 2SiO ₂ sintered material, SiC sintered material, AlN Shitsushoyui Body, Si ₃ N ₄ -based sintered body, and any ceramic material such as a glass ceramic sintered body, a highly heat-resistant resin material such as polyimide, or a material such as glass, or Fe- A metal material such as Ni alloy, Fe—Ni—Co alloy, SUS, Al, Al alloy can be appropriately selected and used.

  Further, the heating resistor layer 5c is preferably a metal member, and has excellent adhesion to the introduction pipe 5a and the lead-out pipe 5b, reducing the loss of power consumption due to heat transfer, and introducing the pipe 5a. In addition, the raw material flowing in the outlet pipe 5b can be heated, and the more efficient reactor 11 can be realized. The metal material preferably has a high electric resistance. For example, Mo-Mn, W, Pt, or the like is used. When Mo—Mn or W is used for the metal introduction pipe 5a and the lead-out pipe 5b, an electrical insulator such as glass or ceramic is used as the lead-in pipe 5a and the lead-out pipe so that the heating resistor layer 5c functions as a heater. It is preferable to interpose between 5b and the heating resistor layer 5c, or to perform an insulation treatment such as oxidizing the surface.

Further, the heating resistor layer 5c can be easily formed on the introduction pipe 5a and the lead-out pipe 5b, and the electrical insulator can be metallized in order to sufficiently function the heating resistor layer 5c as a heating element. It is preferable to use an insulating material that is possible and has excellent adhesion between the introduction pipe 5a and the lead-out pipe 5b and the heating resistor layer 5c. As such an insulating material, ceramic is preferable, and it is possible to provide a heating means by the heating resistor layer 5c without newly providing an electric insulator as described above. As the ceramic material, aluminum oxide _(Al 2 _{O 3)} sintered material, mullite _{(3Al 2 O 3 · 2SiO 2} ) sintered material, silicon carbide (SiC) sintered material, aluminum nitride (AlN) Quality grilled Any of a sintered body, a silicon nitride (Si ₃ N ₄ ) -based sintered body, glass ceramics, and the like can be used.

  Such a heating resistor layer 5c is preferably disposed in the vicinity of the reaction path through which the raw material flows in the reactor 11. Thereby, the heat generated from the heating resistor layer 5c can be efficiently used for the reaction of the raw material. The position in the vicinity of the reaction path is preferably in the range of 0.01 mm to 0.50 mm from the reaction path from the viewpoint of efficiently supplying heat to the reaction path.

(Brazing material)
The brazing material 3 is for airtightly connecting the introduction pipe 5a and the lead-out pipe 5b and the substrate (reactor body) 10. As the brazing material 3 to be used, any one of Ag—Cu, Ag, Au—Ni, Au—Sn, and the like may be appropriately selected depending on the application.

  In connecting the introduction pipe 5a and the lead-out pipe 5b to the substrate (reactor body) 10 by the brazing material 3, the heating resistor layer 5c provided in the lead-in pipe 5a and the lead-out pipe 5b is caused to generate heat and locally heated. By doing so, it is possible to heat and melt only the brazing material 3 through the introduction pipe 5a and the lead-out pipe 5b without heating the entire reactor 11. Therefore, damage to members and the like that may be deteriorated by the high temperature provided in the reactor 11 can be minimized.

(Protective layer)
The brazing material 3 preferably has a protective layer on its surface. Since at least one layer of coating is applied on the brazing material 3, mutual diffusion between the coating layers and the brazing material 3 according to the temperature occurs. When the mutual diffusion occurs, the emissivity of the surface of the brazing material 3 is different. Therefore, by monitoring the power consumption and the emissivity when the emissivity is changed, the introduction pipe 5a and the outlet pipe 5b have a temperature rise or higher than expected. It is possible to confirm that a temperature drop has occurred. As a result, it is possible to safely stop the apparatus and monitor the subsequent progress. The protective layer is preferably subjected to, for example, Au or Ni plating treatment or Al coating treatment so that mutual diffusion is performed. For example, in the case of Au plating treatment, the thickness is preferably 0.1 μm to 5 μm.

(electrode)
Furthermore, the introduction pipe 5 a and the lead-out pipe 5 b are electrically connected to the substrate (reactor body) 10, or are electrically connected to wiring or the like provided in the internal space in the substrate (reactor body) 10. The electrode 7 is provided.

  By providing the electrode 7 on the introduction pipe 5a and the lead-out pipe 5b, the electrode 7 and the heating resistor layer 5c described above can be used together. Further, the heating resistor layer 5c can also be used as a lead terminal 8 for connecting to an external electric circuit.

  For example, as shown in FIGS. 1 and 2, the heating resistor layer 5c formed on each surface of the supply pipe 5a and the lead-out pipe 5b is connected to a bonding wire (not shown). ) Or electrically connected to a substrate (not shown) such as a printed wiring board on which a temperature control device or the like is mounted, for example, through a conductive bonding material, so that power is supplied from the outside.

  Such a temperature adjusting mechanism can heat the heating resistor 5c in a temperature range of about 20 ° C. to 800 ° C. according to the raw material reaction conditions to adjust the inside of the introduction pipe 5a and the outlet pipe 5b to desired temperature conditions. The raw material supplied from the raw material supply port connected to the introduction pipe 5a is preheated so that the chemical reaction is favorably promoted in the substrate (reactor body) 10, or the substrate (reactor body). The chemical reaction of the raw material after the reaction within 10 can be further promoted and discharged from the outlet pipe 5b.

  For example, in order to maintain the reactor 11 at a constant temperature by incorporating a heater or the like in the substrate (reactor main body) 10 and continuously supplying power to the heater, a low heat transfer path length can be used. The reactor 11 capable of operating with power consumption can be realized. From the viewpoint of reducing heat transfer, it is preferable that the thermal conductivity is low and the cross-sectional area is small.

(Body)
The casing 9 in the present invention has a role as a container for storing the reactor 11 in both the substrate 1 and the lid 4.

These include, for example, Fe-based alloys such as stainless steel (SUS), Fe-Ni-Co alloys, Fe-Ni alloys, metal materials such as oxygen-free copper, aluminum oxide (Al ₂ O ₃ ) -based sintered bodies, mullite _{(3Al 2 O 3 · 2SiO 2} ) sintered material, silicon carbide (SiC) sintered material, aluminum nitride (AlN) sintered material, silicon nitride _(Si 3 _{N 4)} sintered material, glass ceramic It is made of a ceramic material such as polyimide, a highly heat-resistant resin material such as polyimide.

  When the casing 9 is made of ceramics, the same material and manufacturing method as those of the introduction pipe 5a and the lead-out pipe 5b described above can be used.

On the other hand, when the housing 9 is made of a metal material, a cutting method, a pressing method, MIM (Metal
It is formed into a predetermined shape by the injection molding method.

  Further, when the casing 9 is made of a metal material, the surface thereof is preferably subjected to coating treatment such as Au or Ni plating or resin coating such as polyimide in order to prevent corrosion. For example, in the case of Au plating treatment, the thickness is preferably 0.1 μm to 5 μm.

  The casing 9 as described above should be thin in order to enable the reactor 11 to be reduced in size and height, but in view of mechanical strength, the bending strength should be 200 MPa or more. preferable.

  And in order to acquire the heat insulation in the reaction apparatus 12, it is preferable to provide a space between the reactor 11 and the housing 9, and to make this space a vacuum. For example, it is preferable that the pressure in the reaction apparatus 12 is less than 100 Pa.

  In order to make the pressure between the reactor 11 and the housing 9 less than 100 Pa, the following method may be mentioned. That is, when the reactor 11 is sealed, it is sealed by a brazing material 3 in a vacuum furnace, a seam weld method in a vacuum chamber, electron beam welding, projection welding, or the like, or in an inert atmosphere in advance. After sealing by seam welding method, projection welding, etc., the reactor is evacuated from a evacuation pipe (not shown) formed in the reactor 12, and the evacuation pipe is crushed and pressure-bonded. What is necessary is just to make the inside of 12 into the said pressure.

  FIG. 3 is a cross-sectional view of a reaction apparatus 12a including a reactor 11a showing another embodiment of the present invention. Note that the same reference numerals are given to the portions corresponding to the above-described embodiment. Compared to the reactor 11 of the above-described embodiment, the reactor 11a of the present embodiment is provided with a heating resistor 5c as heating means only in the introduction pipe 5a, and the heating resistor 5c in the outlet pipe 5b. It is different in that is not provided. Also by adopting such a configuration, similarly to the above-described embodiment, the heating resistor 5c is heated to preheat the raw material, and heated to an optimum temperature into the substrate (reactor body) 10. For example, the raw material can be supplied to the substrate (reactor body) 10 in an activated state.

  Further, in still another embodiment of the present invention, contrary to the reactor 11a of FIG. 3 described above, the heating resistor 5c, which is a heating means, is provided only in the outlet pipe 5b, thereby discharging from the reactor. The raw material after the reaction can be post-heated to further promote the reaction.

It is sectional drawing of the reaction apparatus 12 provided with the reactor 11 which shows one Embodiment of this invention. It is sectional drawing of the reactor 11 shown in FIG. It is sectional drawing of the reaction apparatus 12a provided with the reactor 11a which shows the other form of implementation of this invention.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 Substrate 3 Brazing material 4 Lid 5a Inlet pipe 5b Outlet pipe 5c Heating means (heat generating resistor layer)
7 Electrode 9 Housing 10 Base (Reactor body)
11, 11a reactor 12, 12a reactor

Claims (9)

A substrate having an internal space;
An introduction pipe and a lead-out pipe made of a dielectric material, inserted through the inside and outside of the base body, and joined to the base body via a brazing material;
Heating means provided in the introduction pipe and the outlet pipe;
The reactor characterized by including.   The reactor according to claim 1, wherein the heating means is provided on at least one surface of the introduction pipe and the outlet pipe.   The reactor according to claim 1 or 2, wherein the heating means is provided inside at least one wall of the introduction pipe and the outlet pipe.   The reactor according to any one of claims 1 to 3, wherein the heating means is made of a metal material.   The reactor according to any one of claims 1 to 4, wherein the heating means is made of a metallized material.   The reactor according to any one of claims 1 to 3, wherein at least one of the introduction pipe and the lead-out pipe is made of ceramic.   The reactor according to claim 1, further comprising a protective layer deposited on a surface of the brazing material.   At least one of the introduction pipe and the lead-out pipe has an electrode that is electrically connected to the base body or a conductor provided in an internal space in the base body. The reactor described. A reactor according to any one of claims 1 to 8;
A housing in which the reactor is accommodated and disposed via the reactor and a space;
Comprising
The reactor is characterized in that the pressure in the space is less than 100 Pa.

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