WO2019107401A1

WO2019107401A1 - Microwave treatment device, microwave treatment method, heating treatment method and chemical reaction method

Info

Publication number: WO2019107401A1
Application number: PCT/JP2018/043757
Authority: WO
Inventors: 西岡　将輝; 正人宮川; 麻子鈴木; 優一橋本
Original assignee: 国立研究開発法人産業技術総合研究所; アダマンド並木精密宝石株式会社
Priority date: 2017-11-28
Filing date: 2018-11-28
Publication date: 2019-06-06
Also published as: JP6971812B2; JP2019102142A

Abstract

The present invention provides a microwave treatment device having: a ceramic structure comprising a sintered compact of a laminated ceramic layer; a through hole in the ceramic structure and in which is arranged an object to be treated; and a conductor part that enables propagation of microwaves in the ceramic structure. The microwave treatment device subjects the object to be treated that is arranged in the through hole to a microwave treatment using microwaves supplied to the ceramic structure.

Description

Microwave treatment apparatus, microwave treatment method, heat treatment method and chemical reaction method

The present invention relates to a microwave processing apparatus, a microwave processing method, a heat processing method, and a chemical reaction method.

Microwaves are widely used from household use such as microwave ovens, and then practical development and utilization are being studied as industrial heating systems. By the microwave irradiation, since the object to be treated directly generates heat, it can be heated in a short time, and there is an advantage that temperature unevenness due to heat conduction can be reduced. In addition, there are advantages such as being able to heat without contact and selectively heating only those with good microwave absorption.

Since the energy intensity of the microwave, which is an electromagnetic wave, changes with the wavelength period, heating unevenness easily occurs. For this reason, measures such as irregular reflection of an electromagnetic wave are often performed by moving the position of the object to be processed temporally.
In order to cope with the problem of the uneven heating, it is also considered to use a standing wave of microwaves. For example, Patent Document 1 describes a microwave processing apparatus using a cavity resonator. In this technique, an axisymmetric microwave electric field parallel to the central axis is generated in a cylindrical cavity resonator, and a chemical reaction proceeds in a circular tube disposed in a portion where the electric field strength is concentrated. Further, in Patent Document 2, a flow pipe is disposed along a portion where the electric field strength of the single mode standing wave formed in the cavity resonator is maximized, and the fluid is made to flow by flowing the fluid in the flow pipe. A flow type microwave based chemical reactor that heats rapidly and uniformly is described. Patent Document 3 describes the use of feedback control means for controlling the oscillation frequency of the microwave generator to match the current resonance frequency of the cavity resonator. By this, the resonance state of TM ₀₁₀ is always maintained, and high-precision heat treatment becomes possible.
By using the cavity resonator as described above, a standing wave can be formed inside, and the object to be treated can be heated uniformly and efficiently.

Japanese Patent Application Laid-Open No. 2005-322582 JP, 2010-207735, A JP, 2009-80997, A

However, in the techniques described in the above-mentioned patent documents, in order to form a standing wave of microwaves, the cavity resonator needs to have a certain size. This is because a microwave irradiation area for forming a standing wave according to the wavelength of the supplied microwave is required. If the size of the cavity resonator is large, naturally, miniaturization of the microwave processing apparatus can not be realized. As a result, the application range of the microwave processing apparatus is limited. Here, a cavity resonator refers to a resonator having a space in which no solid filling is present inside the resonator.

An object of the present invention is to reduce the size and weight of a microwave processing apparatus using standing waves.

As a result of intensive investigations in view of the above problems, the present inventors obtained ceramic structure resonators instead of cavity resonators, whereby the wavelength of the microwave necessary for forming a standing wave is sufficient. Can be shortened. As a result, it has been found that the desired standing wave can be formed even if the resonator is miniaturized. Also, it has been found that the function of the cavity resonator can be expressed by forming a conductive pattern in the ceramic structure instead of the cavity made of a metal container in order to form a standing wave. This has the effect of reducing the weight by reducing the metal container.
The present invention has been further studied based on these findings and has been completed.

That is, the above-mentioned subject of the present invention is solved by the following means.
[1]
A ceramic structure comprising a sintered body of laminated ceramic layers;
The ceramic structure includes a through hole in which the object to be treated is disposed, and a conductor portion which enables the microwave to propagate through the ceramic structure.
The microwave processing apparatus which carries out the microwave processing of the said to-be-processed target object arrange | positioned in the said through-hole by the microwave supplied to the said ceramic structure.
[2]
The ceramic structure is a ceramic structure resonator having a portion of the conductor portion that forms a standing wave in its inside,
The microwave according to [1], wherein the through hole is disposed at a position where an electric field or a magnetic field of a standing wave formed in the ceramic structure becomes maximum, and the object to be treated is subjected to microwave treatment by the standing wave Processing unit.
[3]
The microwave processing apparatus according to [1] or [2], wherein the temperature control of the object to be processed is performed by the microwave processing.
[4]
The microwave processing apparatus according to any one of [1] to [3], wherein the object to be treated is heated by the microwave treatment.
[5]
The through holes communicate with the upper and lower surfaces of the ceramic structure,
The conductor portion enables the formation of a standing wave of microwaves in the ceramic structure,
The microwave processing apparatus according to any one of [1] to [4], wherein the object to be treated is heated by the standing wave.
[6]
The conductor portion has an antenna function for introducing microwaves, and an electromagnetic wave shielding function for preventing the microwaves from being dissipated to the outside of the ceramic structure. The microwave processing apparatus described in.
[7]
The microwave processing apparatus according to [6], wherein the conductor portion having the antenna function is an antenna wire disposed inside from outside the ceramic structure and an antenna connected to the antenna wire.
[8]
The microwave processing apparatus according to [6] or [7], wherein a standing wave forming region is defined by the conductor having the electromagnetic wave shielding function.
[9]
The standing wave is in TM 0 _{n 0} mode,
The micro-circuit according to any one of [1] to [8], wherein a plurality of the conductor portions are arranged at intervals in a cylindrical shape or a square cylinder shape on the ceramic structure around the through hole. Wave processing equipment. However, n is a positive integer.
[10]
The microwave according to any one of [1] to [9], wherein the microwave processing apparatus is a chemical reaction apparatus that heats the object to be treated by a standing wave of microwaves to generate a chemical reaction. Processing unit.
[11]
The microwave processing apparatus according to any one of [1] to [10], wherein the object to be treated is a fluid.
[12]
A microwave treatment method comprising treating the object to be treated in the through hole with a microwave using the microwave treatment device according to any one of [1] to [11].
[13]
A heat treatment method comprising heating the object to be treated in the through hole with a microwave using the microwave treatment apparatus according to any one of [1] to [11].
[14]
The object to be treated is a fluid,
[13] The heat treatment method according to [13], including causing one or both of state change of the fluid and a chemical reaction by the heating.
[15]
[14] The heat treatment method according to [14], wherein the state change is a temperature change or a phase change of the fluid.
[16]
A chemical reaction method comprising causing a chemical reaction by microwave treatment of the object to be treated in the through hole using the microwave treatment device according to any one of [1] to [11]. .

The microwave processing apparatus of the present invention can be miniaturized, has a wide range of application, and can be reduced in weight.

The above and other features and advantages of the present invention will become more apparent from the following description with reference to the accompanying drawings as appropriate.

It is the perspective view which showed typically one preferable embodiment of the microwave processing apparatus of this invention. It is an abcd surface schematic sectional drawing of the microwave processing apparatus shown in FIG. It is a top view of the microwave processing apparatus shown in FIG. It is the temperature change figure which showed the result of having measured the change of the water temperature of the distribution pipe exit in the presence or absence of microwave irradiation. It is a temperature change figure showing the result of having measured the temperature change of pure water to microwave input electric power by making the sending speed of pure water into a parameter. It is a temperature change figure showing the result of having measured the temperature change of pure water using the specimen 1 which connected the conductive pattern which provided the upper surface electrode and the lower surface electrode in the side wall of the specimen.

Hereinafter, a preferred embodiment of a microwave processing apparatus of the present invention will be described with reference to the drawings.

[Microwave processor]
A preferred embodiment of the microwave processing device of the present invention will be described with reference to FIGS.
As shown in FIGS. 1 to 3, the microwave processing apparatus 1 applies a microwave to the ceramic structure 11, the through holes 21 disposed in the ceramic structure 11, and part or all of the through holes 21. And the conductor portion 31 of FIG.

The ceramic structure 11 is made of a sintered body of the laminated ceramic layers 12. For the ceramic layer 12, for example, Low Temperature Co-fired Ceramics (LTCC) can be used. There are various types of LTCC, for example, one obtained by mixing a glass component (for example, borosilicate glass) with aluminum oxide (alumina). The “low temperature” is a temperature at which the metal (eg, silver, copper, etc.) used for the wiring and the connection portion is not deformed, deteriorated, or melted, and is, for example, 850 to 1000 ° C. As used herein, the term "ceramic layer" includes sheet, plate and the like. The term "sintered body" also includes those obtained by heating and integrating the laminated ceramic layers. Thus, sintering (firing) can be performed at a temperature considerably lower than the firing temperature (for example, 1500 ° C.) of a general ceramic. Therefore, silver, copper, or the like can be used for the wiring and the like. For example, a paste-like metal (silver paste, copper paste, etc.) can be used.

In the ceramic structure 11, when microwaves are supplied to the standing wave formation region 13, the wavelength of the standing wave formed in the ceramic structure 11 having a dielectric constant higher than that of the cavity is the same as that of the cavity resonator. It becomes shorter than the wavelength of the standing wave formed in the cavity. The standing wave forming region 13 required to form the standing wave can be narrowed, and the ceramic structure 11 can be miniaturized. Thus, the ceramic structure 11 constitutes a resonator (also referred to as a ceramic structure resonator) 2 having a part of the conductor portion 31 that forms a standing wave in the ceramic structure 11.
In order to realize the miniaturization of the resonator 2, the dielectric constant of the ceramic structure 11 is preferably 2 or more, more preferably 4 or more, and still more preferably 7 or more. The ceramic structure 11 also generates heat due to the absorption of microwaves. In order to reduce the influence of the heat generation, the dielectric loss tangent of the ceramic structure 11 is preferably 0.005 or less, more preferably 0.002 or less, and still more preferably 0.001 or less.

Conventional metal cavity resonators are formed using light density aluminum as an example. There is not much difference between the density of aluminum and the density of alumina ceramic. For this reason, when the size of the resonator is equal, the use of alumina ceramic instead of aluminum does not result in significant weight reduction. However, if miniaturization can be realized as in the present invention, significant weight reduction becomes possible, and the range of application is expanded.

The through hole 21 is a hole through which an object to be treated (not shown) passes, and is disposed inside the ceramic structure 11 so as to communicate with the upper and lower surfaces thereof. In the illustrated example, the through holes 21 are formed in a linear shape, but may be formed in a curved shape, for example, a spiral shape or the like. The through hole 21 may be provided with a flow pipe 6 through which an object to be treated is passed. In this case, it is preferable that the through holes 21 have high electric field strength in the direction perpendicular to the direction in which the through holes 21 are arranged, and the electric field strength be uniform in the direction in which the flow pipe 6 is arranged. By arranging such a through hole 21, for example, by matching the flow pipe 6 arranged in the through hole 21 to a portion where the electric field strength is maximized, the object to be treated can be efficiently and rapidly heated. be able to. Further, even if the object to be treated is disposed directly in the through hole 21 without distributing the flow pipe 6 or is circulated, the object to be treated can be efficiently done as in the case of passing the inside of the flow pipe 6 , Can be heated rapidly.

The ceramic structure 11 is designed such that the inside surrounded by the upper surface conductor, the lower surface conductor and the post wall conductor connected to the upper surface electrode (not shown) and the lower surface electrode (not shown) acts as a resonator It is done. The upper surface conductor is the conductor portion 31B on the surface on the ab line side, and the lower surface conductor is the conductor portion 31B on the surface on the cd line side. The post wall conductors are a plurality of spaced apart annular conductive portions 31 B connected to the upper surface electrode (not shown) and the lower surface electrode (not shown). A portion including all of these conductor portions is referred to as a conductor portion 31. Further, a portion of the ceramic structure 11 acting as a resonator is referred to as a ceramic structure resonator 2.
The conductor portion 31 has an antenna function for introducing microwaves, and an electromagnetic wave shielding function for preventing the microwaves from being dissipated to the outside of the ceramic structure resonator 2.
The conductor portion 31 (31A) having the antenna function includes the antenna wire 41 disposed on the inner side from the outer wall side of the ceramic structure 11, the antenna 43 serving as a microwave supply port, and the ground wire 44 of the antenna 43. Have. Therefore, the antenna 43 is disposed on the outer peripheral side in the standing wave forming area 13 described later. A standing wave is formed in the standing wave formation region 13 by the microwave supplied from the antenna 43.
A plurality of conductor portions 31 (31 B) having an electromagnetic wave shielding function are disposed annularly at intervals in the ceramic structure resonator 2 around the through holes 21. The term "annular" is used to mean including a cylindrical or square cylinder. The “spaced” means that the conductor portions 31 are spaced apart, and means, for example, equally spaced or arbitrarily defined intervals. The conductor portion 31 B is formed in a rod-like body so as to be in communication with the upper and lower surfaces of the ceramic structure resonator 2. In the illustrated example, the portion surrounded by the plurality of conductor portions 31B arranged in a cylindrical shape at intervals is the standing wave forming region 13, and the portion including the conductor portion 31 is a resonator. Moreover, in order to separate the standing wave formation area 13 to which microwaves are supplied from the external world, the electromagnetic shield of the standing wave formation area 13 is provided by providing the conductor portion 31B so as to surround the standing wave formation area 13. Is made. The distance between each conductor portion and the adjacent conductor portion is preferably narrow, but is not particularly limited as long as it is sufficiently shorter than the wavelength of the electromagnetic wave formed inside the ceramic, and the desired standing wave is formed in the standing wave forming region 13 It can be set appropriately in consideration of the type of ceramic and the microwave frequency so as to be able to.
Volume ceramic structure resonator 2 is that bounded by the conductor portion 31B, preferably 0.5 ~ 30 cm ³ or less, more preferably 1.0 ~ 8.0 cm ^3, for example, 1.0 ~ 3.0 cm ³ It can be done. In the case of a conventional cavity resonator (microwave frequency is 2.45 GHz), a length of approximately 12 cm is required to form a standing wave, and the volume of the resonator is 180 cm ³ or more.

By the configuration of the conductor portion 31, a microwave (a standing wave) is irradiated to a part or the whole of the through hole 21. At this time, the standing wave forming area 13 is defined by the conductor portions 31B arranged in a ring shape spaced apart from each other. For example, when the conductor portion 31B is disposed in a cylindrical shape, the distance between the cylindrical conductor portions 31B facing in the radial direction may be set to, for example, the wavelength of the microwave in which the standing wave is formed. preferable.

In the ceramic structure resonator 2, the energy of the standing wave formed in the resonator is maximal in the direction of the through hole 21 (also referred to as the central axis C direction), and the energy of the standing wave is in the central axis C direction It becomes uniform. In such a through hole 21, the flow pipe 6 penetrating the through hole 21 can be disposed. In this case, the object to be treated is disposed in the flow pipe 6. For example, in the case of the ceramic structure resonator 2 in which the conductor portion 31B is disposed in a cylindrical shape at intervals so as to generate a standing wave of TM ₀ n ₀ mode (n is an integer of 1 or more), the cylindrical center The electric field intensity of the axis C becomes maximum, and the electric field intensity becomes uniform along the central axis C. For this reason, it is preferable that the through holes 21 through the flow pipe 6 be disposed on the central axis C of the cylindrical shape.

The ceramic structure resonator 2 is provided with the microwave generator 5 (see FIG. 1), and the microwave generator 5 is connected to the ceramic structure resonator 2 through the cable 45, the antenna wire 41 and the antenna 43. Microwaves are supplied into the standing wave forming region 13. In general, an S band centered on 2.45 GHz is used as the microwave frequency.

In the microwave processing apparatus 1 described above, the flow pipe 6 is disposed inside the through hole 21 as necessary. An object to be treated (not shown) is present in the through hole 21 or the flow pipe 6, or the object to be treated flows through the ceramic structure resonator 2. A wave is supplied to form a standing wave in the standing wave forming region 13 in the resonator. If the through hole is provided along the portion where the electric field strength of the standing wave is maximized, the object to be treated in the through hole 21 or the flow pipe 6 can be efficiently and rapidly heated. In the microwave processing apparatus 1, microwaves forming a standing wave are supplied from the antenna 43 provided in the ceramic structure resonator 2 into the resonator.

In the microwave processing apparatus 1, the microwaves supplied from the microwave generator 5 are adjusted in frequency and supplied. By adjusting the frequency, the electric field strength distribution of the standing wave formed in the ceramic structure resonator 2 can be controlled to a desired distribution state, and the strength of the standing wave can be adjusted by the output of the microwave. That is, it is possible to control the heating state of the object to be treated.
In addition, the frequency of the microwave supplied from the antenna 43 can form a specific single mode standing wave in a resonator.
The structure of the microwave processing apparatus 1 of this invention is demonstrated in order.

<Resonator (Ceramic Structure Resonator)>
The shape of the ceramic structure resonator (cavity) 2 used in the microwave processing apparatus 1 has one microwave supply antenna 43, and when a microwave is supplied, a single mode standing wave is formed There is no particular limitation as long as For example, it is possible to use the ceramic structure resonator 2 in which the conductor portions 31 are arranged at intervals in a cylindrical or rectangular shape. In the present specification, the term “cylindrical” is used to mean one having a circular cross-sectional shape perpendicular to the central axis C of the resonator, as well as one having an elliptical or oval cross-sectional shape. In addition, the term “square cylinder” means that the cross-sectional shape perpendicular to the central axis C is a polygon, and the cross-sectional shape is preferably a quadrilateral to a dodecagonal shape. Also, the corners of the polygon may have a rounded shape. In the case of a polygon, if there are more corners, it can be approximated to a cylindrical shape.
It is desirable that the size of the ceramic structure resonator 2 is also small as long as a standing wave can be formed, but the size can be appropriately designed according to the purpose. The resonator preferably has a high dielectric constant, and is preferably made of ceramic. As an example, LTCC can be used. The LTCC is a mixture of aluminum oxide (alumina) and a glass component (for example, borosilicate glass). Moreover, the metal paste mentioned above can be used for the conductor part 31 (31A, 31B). Furthermore, the surface of the ceramic structure resonator 2 may be coated with a substance having a low electrical resistivity by plating, vapor deposition or the like. It is preferable to use a material containing silver, copper, gold, tin and rhodium for the coating.

<Supply of microwaves>
The microwave processing apparatus 1 of the present invention is an apparatus suitable for performing the above-described heating control. A microwave processing apparatus 1 comprises a ceramic structure resonator 2 having an antenna 43 for supplying microwaves, and a micro-wave for supplying microwaves of a frequency at which a standing wave can be formed in the resonator. And a wave generator 5. The microwave generator 5 is also preferable as a configuration including a microwave amplifier (not shown).
The structure of the resonator which comprises the microwave processing apparatus 1 of this invention is the same as what was demonstrated by the above-mentioned "resonator."

As the microwave generator 5, for example, a microwave generator such as a magnetron or a microwave generator using a solid semiconductor element can be used. It is preferable to use a microwave generator using a solid semiconductor device from the viewpoint of compactness and fine adjustment of the frequency of the microwave.

As shown in FIGS. 1 to 3, in the microwave processing apparatus 1, in the ceramic structure 11, a ceramic in which a plurality of conductor portions 31 </ b> B are arranged at equal intervals along the cylindrical side wall defining the resonator. The structure resonator 2 can be used. The inside of this cylindrical shape is the standing wave forming area 13. A microwave supply antenna (also referred to simply as an antenna) 43 is provided in a plane parallel to the central axis C of the resonator (the inner surface of the cylindrical shape) or in the vicinity thereof. In one embodiment, the antenna 43 is an antenna to which a high frequency can be applied, and a magnetic field excitation antenna, for example, a loop antenna is preferably used. The antenna 43 is connected to the antenna wire 41 provided in the ceramic structure resonator 2, and is further connected to the microwave generator 5 through the cable 45 electrically connected to the antenna wire 41. As the cable 45, for example, a coaxial cable is used. In this configuration, the microwaves emitted from the microwave generator 5 are supplied from the antenna 43 into the standing wave forming region 13 of the resonator via the cable 45 and the antenna wire 41. Between the microwave generator 5 and the antenna 43, a matching device (not shown) for suppressing a reflected wave or an isolator (not shown) for protecting the microwave generator may be installed.
The other end of the antenna 43 is connected to a ground potential such as a resonator wall through a ground line 44. By applying a microwave (high frequency) to the antenna 43, a magnetic field is excited in the loop to form a standing wave in the standing wave forming region 13 in the resonator.
For example, in the resonator having the above-mentioned cylindrical standing wave forming region 13, when forming a single mode standing wave of TM ₀₁₀ , the electric field strength becomes maximum at the central axis C, and in the central axis C direction The electric field strength becomes uniform. Therefore, in the through holes 21 to the flow pipe 6, it is possible to perform microwave heating uniformly and efficiently on the object to be treated which exists or flows inside.

<Heating of the object to be treated>
In the microwave processing apparatus of the present invention, the object to be treated (for example, the object to be treated that is present or circulates in the flow pipe 6) is subjected to microwave treatment in the ceramic structure resonator 2. That is, the object to be processed is disposed at a position where the electric field strength is high corresponding to the electric field strength in the resonator. In particular, if the object to be processed is disposed along the portion where the electric field strength of the standing wave formed in the resonator is maximum, more efficient heating is possible.
Alternatively, the object to be treated may be disposed in a portion where the magnetic field strength is high in correspondence with the magnetic field strength inside the ceramic structure resonator 2. In particular, if the magnetic field strength formed in the resonator is located at a maximum position, more efficient heating is possible. For example, in the case where the object to be treated is a magnetic substance, the absorption of magnetic field energy results in more efficient heating. In the case where the object to be treated is a substance containing metal, ion, or the like and has electrical conductivity, heat can be generated by Joule heat generated by a current excited in the substance by a magnetic field, which enables more efficient heating.
Moreover, when the thickness of the ceramic structure resonator 2 is thin, it is also possible to connect a plurality of resonators in series in the central axis direction. It is also possible to stack two or more and several thousand or so resonators to be connected.

In the microwave processing apparatus 1 shown in FIGS. 1 to 3, the object to be treated disposed in the flow pipe 6 is not particularly limited, and examples thereof include liquids, solids, powders and mixtures thereof. Or the honeycomb structure, the catalyst, etc. which were beforehand installed in the distribution pipe can be mentioned.
When the object to be treated is a fluid, heating of the object to be treated by microwave irradiation may be used to cause one or both of a change in state of the fluid and a chemical reaction. State change includes temperature change or phase change of fluid.
When the object to be treated is liquid, solid, or powder, the object to be treated which has been subjected to the heat treatment can be continuously taken out by conveying it into the flow pipe with a pump or the like. The microwave processing apparatus of the present invention can be used to control chemical reactions because many chemical reactions can control the progress of the reaction by temperature.
When the object to be treated is a honeycomb structure, the microwave processing apparatus can be used, for example, to control the temperature of the gaseous substance passing through the honeycomb structure. Moreover, when using a to-be-processed target object as a catalyst, it can be used in order to produce the chemical reaction by the effect | action of a catalyst so that it may mention later. The catalyst is also preferably supported on a honeycomb structure.
As the chemical reaction, transfer reaction, substitution reaction, addition reaction, cyclization reaction, reduction reaction, oxidation reaction, selective catalytic reduction reaction, selective oxidation reaction, racemization reaction, cleavage reaction, catalytic decomposition reaction (cracking), etc. Are exemplified, but not limited thereto, various chemical reactions may be mentioned.
Specific examples of the chemical reaction include a reaction of oxidizing and decomposing volatile organic substances, a reaction of reducing nitrogen oxides to nitrogen and oxygen, a reaction of fixing sulfur oxides on calcium, a reaction of lightening heavy oil, etc. It can be mentioned.

In the chemical reaction method of the present invention, conditions such as reaction time, reaction temperature, reaction substrate, reaction medium and the like may be appropriately set according to the target chemical reaction. For example, Handbook of Chemistry (Shuichi Suzuki, Mitsuaki Mukayama, Asakura Shoten, 2005), Microwave Chemistry Process Technology II (Kazuhiko Takeuchi, Yuji Wada, CMC Publishing, 2013), JP 2010-215677, etc. The chemical reaction conditions can be set appropriately, referring to.

In the embodiment shown in FIG. 1, the frequency of the standing wave is not particularly limited as long as the standing wave can be formed in the resonator. For example, it can be a frequency from the antenna 43 when supplying microwaves, which the ceramic structure in the resonator 2 standing waves TM _0n0 mode or TE _10n mode is formed for supplying microwaves. However, n is a positive integer.
Standing wave of the _{TM 0n0} mode, for example _TM _010, TM _020, include mode _{TM 030,} it is preferably a standing wave of inter alia _{TM 010.}

Next, an example of a method of manufacturing the ceramic structure resonator will be described below.
The LTCC is formed into a sheet to the size of the ceramic structure of the ceramic structure resonator. The number of moldings is the number of laminated ceramic layers forming the ceramic structure. One of the ceramic layers has a thickness of 0.01 mm to 0.3 mm, preferably 0.035 mm to 0.13 mm, more preferably 0.1 mm to 0.13 mm. Have.
By subjecting the formed sheet to a punching process using a laser beam, a through hole and a hole for a conductor forming the conductor portion are formed. The through holes are formed in the center of the standing wave formation region, and cylindrical and equidistantly spaced holes for conductor for the cavity pattern for TM ₀₁₀ are formed around the through holes. Further, in a layer for forming an antenna, a groove for forming an antenna line and a groove for forming an antenna for microwave irradiation are formed. Further, in the required ceramic layer, a grounding wire hole grounded from the antenna is formed.
Next, the inside of each hole and each groove is filled with a conductive material. For example, it is preferable to fill with silver paste, copper paste or the like.
In addition, it is also preferable to form an antenna and an antenna wire by printing of a conductive pattern. In that case, it is preferable to carry out after the above-mentioned filling. That is to ensure connection between the conductive material filled in the holes and the conductive pattern formed by printing.
Next, a ceramic layer is laminated so as to form a ceramic structure. At that time, they are aligned and stacked so that the conductor portions formed in the holes and the like are connected to each other. For example, in the case of forming a microwave processing apparatus having a thickness of 5 mm, 30 to 50 ceramic layers are laminated.
Moreover, it is also preferable to coat the surface of the laminate with a conductive material, if necessary.
Thereafter, the laminated ceramic layers are sintered and joined. In the present specification, laminating ceramic layers such as ceramic sheets and bonding them by heat is also a category of sintering.
The sintering temperature is 850 ° C. to 1000 ° C., and silver, copper and the like of the metal used for the wiring and the connection portion do not deteriorate or melt. Therefore, sintering can be performed while maintaining the shapes of the wiring and the connection portion. In addition, the sintered body is formed into the size of the ceramic structure 11 by cutting, grinding or the like, as necessary. Alternatively, it may be formed to the size of the ceramic structure 11 and then sintered.
In addition, if necessary, a conductive pattern for a detector for detecting standing waves is printed on the surface of the sintered ceramic structure. Moreover, it is also preferable to perform a plating process. In this way, a ceramic structure is formed and can function as a ceramic structure resonator.
Based on the above-mentioned manufacturing method, a ceramic structure resonator was made on a trial basis. When microwaves were supplied to this ceramic structure resonator, it was possible to control the heating of the liquid passing through the through hole. The present ceramic structure resonator has a mass and volume less than 1/10 that of the conventional metal cavity resonator.

In addition, the microwave processing apparatus 1 can heat an object to be treated through the through hole or an object to be treated through the flow pipe, or cause a chemical reaction. Alternatively, gas can be passed through the flow tube to generate plasma.

The microwave processing apparatus 1 is preferably designed such that the resonance frequency of the ceramic structure resonator 2 falls within the industrially available ISM band. In addition, since the resonance frequency fluctuates due to the temperature change and the composition change of the object to be treated, it is preferable that the resonance frequency falls within the ISM band in consideration of the fluctuation range. “ISM” is an abbreviation of Industry Science Medical, and the ISM band is a band of frequencies assigned for general use in the industrial, scientific and medical fields.

When the ceramic structure resonator 2 is formed of a ceramic layer, it is preferable to use a ceramic layer having a small dielectric loss. When a ceramic layer having a small dielectric loss is used, microwaves are less likely to be absorbed by the ceramic layer, and the heat generation of the ceramic structure resonator 2 can be suppressed. Thereby, the heating efficiency of a to-be-processed target object can suppress a fall. In addition, it is possible to suppress the risk of inducing troubles such as thermal transformation or ignition of the dielectric.

The ceramic structure resonator 2 of the microwave processing apparatus 1 can realize a significant reduction in size and weight as compared with the conventional cavity resonator.
As described above, since miniaturization and weight reduction can be realized, the microwave processing apparatus can be integrally formed with another apparatus. For example, the applicability to disposable applications such as medical fluid temperature control in the medical field is broadened.

Furthermore, in the above-mentioned microwave processing apparatus, the following effects can also be mentioned.
(1) The small size increases the energy density and enables high-temperature heating more quickly. Therefore, the scope of application extends to various chemical reactions, including the synthesis of chemical materials.
(2) It is possible to supply sufficient microwave energy to the object to be treated even by using a relatively inexpensive low-power microwave generator. Therefore, the device price can also be reduced.
(3) The number of microwave generators and ceramic structure resonators can be increased or decreased stepwise according to the increase or decrease of production scale, so that various production modes can be flexibly coped with.
(4) It is possible to incorporate a desired function such as installing a detector in the ceramic structure resonator. Therefore, for example, since it becomes possible to detect the standing wave by the detector and adjust the frequency of the microwave by the microwave generator, the resonator can be controlled, for example, the microwave irradiation condition and the heating condition in the resonator. it can. As a result, fine temperature control of the object to be treated in the distribution pipe is possible.

Hereinafter, the present invention will be described in more detail based on examples, but the present invention is not construed as being limited thereto.

Example 1
As a test body A, the microwave processing apparatus 1 shown in FIGS. 1 to 3 was manufactured based on the above-described manufacturing method. The ceramic structure resonator 2 is a ceramic structure in which ceramic layers 12 made of LTCC are laminated (35 to 40 layers) and sintered to construct a TM ₀₁₀ resonator (cavity). The ceramic layer 12 having a dielectric constant of 7.8 and a dielectric loss tangent of 0.002 was used for the LTCC. Further, in the ceramic layer 12, 16 conductor portions 31B having a diameter of 0.1 to 0.3 mm were previously arranged at equal intervals cylindrically around the through holes 21 having a diameter of 3 mm. In addition, when the ceramic structure resonator 2 is manufactured, the antenna 43 for supplying microwaves, the antenna wire 41, the ground wire 44, and the antenna or antenna wire of a detector not shown are provided in advance on the ceramic layer 12. It produced simultaneously. As a result, a miniaturized ceramic structure resonator 2 having a volume of 8 cm ³ (4 cm × 4 cm × 0.5 cm) and a mass of 25 g was obtained. On the other hand, the conventional cavity resonator had a volume of 200 cm ³ (10 cm × 10 cm × 2 cm) and a mass of 1.3 kg. As described above, the microwave processing apparatus 1 of the present invention can achieve size reduction and weight reduction.
An SMA terminal is attached to each of the microwave (power) supply antenna 43 and the detector antenna (not shown) of the test body A prepared above, and a network analyzer (E5071C (trade name) manufactured by Agilent Co., Ltd.) is used. The S21 signal was measured. The port 1 of the network analyzer is a power supply antenna, and the port 2 is a detector antenna.
When the spectrum of the S21 signal of the test body A was examined, it was found that the S21 signal was -29.2 dB at a frequency of 2.40825 GHz, and a TM ₀₁₀ mode standing wave could be formed.

Next, in the test body A described above, a tetrafluoroethylene (for example, Teflon (registered trademark)) tube is used as the flow pipe 6 having an outer diameter of 2 mm and an inner diameter of 1 mm in a state of penetrating the central axis C of the through hole 21 of the test body A I inserted the flow tube of. As a result, the resonant frequency of the S21 signal shifted to the lower side of 2.407438 GHz. From this, it was confirmed that the formed standing wave (electromagnetic wave) interacts with that supplied to the through hole 21 portion. It was found that the S21 signal was -29.2 dB at a frequency of 2.407438 GHz. The S21 signal does not change before and after tube insertion, which indicates that there is little microwave absorption due to the low dielectric loss of Teflon. Furthermore, when water was fed into the flow pipe 6, the resonance frequency of the S21 signal was further shifted to a lower frequency side, and became 2.391188 GHz. At this frequency, it was found that the S21 signal was -30.5 dB. It becomes clear that the water sent out absorbs the formed standing wave (electromagnetic wave), and this absorbed component causes the heat generation of the water and enables temperature control.

Next, a silicon tube (outer diameter 2 mm, inner diameter 1 mm) was inserted into the through hole 21 of the above test body A as a flow pipe 6 to obtain a test body B. While supplying pure water in the range of 1 mL / h to 60 mL / h with a liquid feed pump (not shown) to this silicon tube, microwaves matching the resonance frequency are supplied from the antenna 43 on the power supply side to 0 W to 90 W In the range of The resonance frequency was investigated by finely adjusting the irradiation frequency so that the signal of the detector antenna (not shown) becomes maximum. We performed feedback control to perform these controls automatically, and built a system to be able to supply microwaves of a predetermined power that always matches the resonance frequency. The temperature of the supplied pure water was measured with a 0.5 mm-thick ultrafine thermocouple (Taka 35 T-35, K 0.5 φ × 100) attached inside a silicon tube. The tip temperature measuring unit of the thermocouple was disposed at a position 1 mm away from the outlet of the flow tube 6 of the silicon tube. The temperature rise ΔT was the liquid temperature before microwave application and the temperature after 10 seconds after microwave irradiation. The microwave input power ΔP is an effective power obtained by subtracting the reflected wave power from the incident wave power of the antenna 43 on the power supply side.

As a post wall conductor (conductor portion 31B) of the test body C, a test body in which 32 conductor portions 31B were arranged at equal intervals in a cylindrical shape around the through hole 21 was used. The feed rate of pure water was 6 mL / h. The time change of the temperature when 17 W is supplied as the input power to the test body C is shown in FIG. The temperature was 19.8 ° C. before the supply of the microwave, but when the microwave was irradiated at the timing of 0 seconds, the temperature rose immediately and became 15 ° C. after 15 seconds. In addition, when the microwave irradiation was stopped after 120 seconds, a temperature drop was observed. From this, it was confirmed that the temperature rise within the microwave irradiation time was due to the heat generation due to the microwave absorption of pure water.

Assuming that the temperature rise due to the microwave irradiation is ΔT, the value of ΔT when the feed rate of pure water was changed in the range of 1 mL / h to 60 mL / h and the microwave input power in the range of 0 W to 17 W was examined. The results are shown in FIG. It was found that by adjusting the microwave input power according to the flow rate of pure water, it is possible to adjust the temperature of pure water.

An example using another ceramic structure resonator as the test body D is shown. That is, in order to enhance the conductivity of the upper surface electrode and the lower surface electrode, a test body having a conductive pattern (not shown) formed on the side wall of the test body C was used. However, the conductive pattern is not formed around the microwave supplying antenna 43 and the detector antenna (not shown), and electrical insulation is maintained. The result of measuring the temperature rise of the pure water similarly flowing through the silicon tube (outside diameter 2 mm and inside diameter 1 mm) of this test body is shown in FIG. In this case as well, it was confirmed that the temperature control of pure water was possible by the microwave input power.

While the present invention has been described in conjunction with its embodiments and examples, it is not intended to limit our invention in any detail of the description unless otherwise specified, and the spirit of the invention as set forth in the appended claims. We believe that it should be interpreted broadly without violating the scope.

The present application claims priority based on Japanese Patent Application No. 2017-228475 filed in Japan on November 28, 2017, which is incorporated herein by reference in its entirety. Capture as part.

1 microwave processing apparatus 2 resonator (ceramic structure resonator)
DESCRIPTION OF SYMBOLS 5 Microwave generator 6 Distribution pipe 10 Microwave irradiation apparatus 11 Ceramic structure 12 Ceramic layer 21 Through-

hole

31, 31A, 31B Conductor part 41 Antenna wire 43 Antenna 44 Ground wire 45 Cable

Claims

A ceramic structure comprising a sintered body of laminated ceramic layers;
The ceramic structure includes a through hole in which the object to be treated is disposed, and a conductor portion which enables the microwave to propagate through the ceramic structure.
The microwave processing apparatus which carries out the microwave processing of the said to-be-processed target object arrange | positioned in the said through-hole by the microwave supplied to the said ceramic structure.
The ceramic structure is a ceramic structure resonator having a portion of the conductor portion that forms a standing wave in its inside,
The microwave according to claim 1, wherein the through hole is disposed at a position where an electric field or a magnetic field of a standing wave formed in the ceramic structure is maximized, and the object to be treated is subjected to a microwave treatment by the standing wave. Processing unit.
The microwave processing apparatus according to claim 1, wherein the temperature control of the object to be processed is performed by the microwave processing.
The microwave processing apparatus according to any one of claims 1 to 3, wherein the object to be treated is heated by the microwave treatment.
The through holes communicate with the upper and lower surfaces of the ceramic structure,
The conductor portion enables the formation of a standing wave of microwaves in the ceramic structure,
The microwave processing apparatus according to any one of claims 1 to 4, wherein the object to be treated is heated by the standing wave.
The said conductor part has an antenna function for introduce | transducing a microwave, and an electromagnetic wave shielding function for preventing that a microwave is dissipated to the exterior of the said ceramic structure. The microwave processing apparatus as described in a term.
7. The microwave processing apparatus according to claim 6, wherein the conductor portion having the antenna function is an antenna wire disposed inside the ceramic structure from the outside and an antenna connected to the antenna wire.
The microwave processing apparatus according to claim 6, wherein a standing wave forming region is defined by the conductor portion having the electromagnetic wave shielding function.
The standing wave is in TM 0 n 0 mode,
The micro tube according to any one of claims 1 to 8, wherein a plurality of the conductor portions are arranged in a cylindrical shape or a rectangular tube shape at intervals in the ceramic structure around the through hole. Wave processing equipment. However, n is a positive integer.
The microwave according to any one of claims 1 to 9, wherein the microwave processing apparatus is a chemical reaction apparatus that heats the object to be processed by a standing wave of microwaves to generate a chemical reaction. Processing unit.
The microwave processing apparatus according to any one of claims 1 to 10, wherein the object to be treated is a fluid.
A microwave treatment method comprising treating the object to be treated in the through hole with a microwave using the microwave treatment device according to any one of claims 1 to 11.
A heat treatment method comprising heating the object to be treated in the through hole by microwave using the microwave treatment apparatus according to any one of claims 1 to 11.
The object to be treated is a fluid,
The heat treatment method according to claim 13, comprising causing one or both of a state change of the fluid and a chemical reaction by the heating.
The heat treatment method according to claim 14, wherein the state change is a temperature change or a phase change of the fluid.
A chemical reaction method comprising causing a chemical reaction by microwave treatment of the object to be treated in the through hole using the microwave treatment device according to any one of claims 1 to 11. .