WO2010116440A1

WO2010116440A1 - Reactor

Info

Publication number: WO2010116440A1
Application number: PCT/JP2009/056447
Authority: WO
Inventors: 靖史松尾; 晃一竹村; 和之湯舟; 誠松倉; 孝夫竹内; 裕介和久田
Original assignee: 電気化学工業株式会社
Priority date: 2009-03-30
Filing date: 2009-03-30
Publication date: 2010-10-14
Also published as: JPWO2010116440A1; JP5539967B2

Abstract

Disclosed is a reactor having high heat insulation and excellent durability, which enables stable production of trichlorosilane. The reactor comprises a generally cylindrical outer-cylindrical-container main body having a bottom plate; an outer-cylindrical-container top cover for hermetically sealing the outer-cylindrical-container main body; a reaction chamber for producing a gas containing trichlorosilane and hydrogen chloride, which is contained in the outer-cylindrical-container main body and into which a gas containing tetrachlorosilane and hydrogen is supplied; a top-cover heat insulation layer covering the inner surface of the outer-cylindrical-container top cover, and a brick layer arranged on the inner surface of the outer-cylindrical-container main body. The brick layer has a multilayer structure wherein a low thermally conductive outermost brick layer and a highly heat-resistant innermost brick layer are arranged in this order from the inner surface of the outer-cylindrical-container main body toward the center thereof.

Description

Reactor

The present invention relates to a reactor for performing a gas phase reaction under a high temperature condition. In particular, the present invention relates to a reactor for trichlorosilane that converts tetrachlorosilane and hydrogen into trichlorosilane.

Trichlorosilane is expected to increase in demand as a raw material gas for high-purity silicon used in elements such as semiconductors and solar cells, and there has been a demand for efficient production of these.

Generally, trichlorosilane (SiHCl3) used as a raw material for producing high-purity silicon (Si: silicon) is produced by reacting tetrachlorosilane (SiCl4: silicon tetrachloride) with hydrogen and converting it. To do.

That is, trichlorosilane is produced by a conversion reaction according to the following reaction formula (1).
SiCl4 + H2 → SiHCl3 + HCl (1)
This reaction is performed by heating a raw material gas composed of gasified tetrachlorosilane and hydrogen to about 800 ° C. to about 1300 ° C. in a reaction furnace.

As described above, since the generation of trichlorosilane is performed in a high temperature environment, the trichlorosilane manufacturing apparatus is provided with a heat insulating structure for preventing heat transfer to the outside.

For example, in Patent Documents 1 and 2, a reaction vessel in which a supply gas of tetrachlorosilane and hydrogen is supplied to the inside and a reaction product gas of trichlorosilane and hydrogen chloride is generated by a conversion reaction, and the periphery of the reaction vessel A heating mechanism for heating the reaction vessel, a heat insulating material arranged to cover the periphery of the reaction vessel and the heating mechanism, and a storage container for storing the reaction vessel, the heating mechanism, and the heat insulating material. An apparatus for producing chlorosilane is disclosed.
The heat insulating material is formed of carbon and attached to the inner wall surface of the cylindrical wall, the upper surface of the bottom plate portion, and the lower surface of the top plate portion so as to be attached inside the storage container, and heat is transferred to the outside of the storage container. The movement is restrained.
JP 2008-133168 A JP 2008-133175 A

Summary of the Invention

In order to efficiently produce trichlorosilane, it is important to perform heating under constant temperature control, and for that purpose, a heat insulating structure capable of maintaining the inside of the reaction vessel at a desired temperature is required.
However, in the heat insulating structures such as Patent Documents 1 and 2, only a single carbon heat insulating material is attached to the inner surface of the storage container, and the top plate of the reaction container is connected to the top plate of the storage container. Since they are in contact with each other, there is a problem that heat insulation is insufficient.

Also, in order to efficiently produce trichlorosilane, a long gas flow path for realizing a sufficient conversion reaction is required, and a large reaction vessel is used. For this reason, when the reaction vessel becomes large and its weight increases, a member that supports the reaction vessel is required to have not only heat insulation performance but also high strength and a long life.

In the trichlorosilane production apparatus of Patent Document 1, the bottom of the reaction vessel is supported by a connecting pipe for gas supply and discharge. Moreover, in the trichlorosilane manufacturing apparatus of patent document 2, the reaction container is supported by the support pillar member installed in the container center part.
However, in such a structure in which the reaction vessel is supported only by the tubular or columnar member, a load due to the weight of the reaction vessel is locally applied to the tubular or columnar member and the bottom of the reaction vessel, which causes damage due to long-term use. It might be.

The present invention has been made in view of the above circumstances, and provides a reactor having high heat insulating properties, capable of producing stable trichlorosilane, and excellent in durability.

According to the present invention, a substantially cylindrical outer cylinder container main body having a bottom plate, an outer cylinder container upper lid that hermetically seals the outer cylinder container main body, the outer cylinder container main body accommodated in the tetrachlorosilane, A reaction vessel in which a gas containing hydrogen is supplied and a gas containing trichlorosilane and hydrogen chloride is generated, an upper lid heat insulating layer that covers the inner surface of the upper cover of the outer cylinder, and an inner surface of the outer cylinder body A laminated structure in which a brick layer is laminated in the order of an outer brick layer with low thermal conductivity and an inner brick layer with high heat resistance from the inner surface of the outer cylinder container main body toward the center. A reaction furnace is provided.

Here, the outermost brick layer having low thermal conductivity means the outermost brick layer composed of bricks having lower thermal conductivity than the brick constituting the innermost brick layer. Moreover, a high heat-resistant innermost brick layer means the innermost brick layer comprised by the brick whose highest use temperature is higher than the brick which comprises an outermost brick layer.

According to the reactor having the above-described configuration, the main body of the outer cylinder container is provided with a main body heat insulating layer and a brick layer, and the brick layer has a plurality of types of brick layers having different properties, i.e., the lowest thermal conductivity. Since it has the laminated structure laminated | stacked in order of the outer brick layer and the innermost brick layer of high heat resistance, heat insulation can be improved remarkably compared with the case where it consists only of a single heat insulating material.

The reactor according to the present invention has high heat insulation, can produce stable trichlorosilane, and is excellent in durability.

1 is a schematic view of a reaction furnace according to the present invention. Sectional drawing of the main body heat insulation layer and brick layer (3 layer structure) provided inside the outer cylinder container main-body part which concerns on this invention. The front view of the stationary plate of the reaction container which concerns on this invention.

Explanation of symbols

DESCRIPTION OF SYMBOLS 101: Reaction furnace 102: Outer cylinder container main-body part 103: Outer cylinder container bottom part 104: Outer cylinder container upper cover part 105: Reaction container 106: Upper cover heat insulation layer 107,202: Main body heat insulation layer 108: Brick layer 109, 300: Fixed plate 110: Gas introduction opening 111: Reaction product gas extraction opening 112: Heater 201: Side wall 203 of outer cylinder container: Outermost brick layer 204: Intermediate brick layer 205: Inner brick layer

BEST MODE FOR CARRYING OUT THE INVENTION

Hereinafter, specific embodiments of the reactor according to the present invention will be described with reference to the drawings.
As shown in FIGS. 1 and 2, the reaction furnace 101 according to the present embodiment includes a substantially cylindrical outer cylinder container main body 102 having a bottom plate (outer cylinder container bottom 103) and an outer cylinder container main body 102 in an airtight manner. A reaction in which a gas containing tetrachlorosilane and hydrogen is supplied to the inside, and a gas containing trichlorosilane and hydrogen chloride is generated by being accommodated in the outer cylinder container upper lid portion 104 and the outer cylinder container main body portion 102 that are sealed to each other. A container 105, an upper lid heat insulating layer 106 covering the inner surface of the outer cylinder container upper lid portion 104, and a brick layer 108 disposed on the inner surface of the outer cylinder container main body portion 102. 2 is a reactor having a laminated structure in which an outermost brick layer (203 in FIG. 2) with low thermal conductivity and an innermost brick layer (205 in FIG. 2) with high heat resistance are laminated in this order from the inner surface to the center. .

The reaction furnace 101 includes a main body heat insulating layer 107 that covers the inner surface of the outer cylindrical container main body 102, a gas introduction opening 110 for supplying gas into the reaction container 105, and a tricycle generated in the reaction container 105. A reaction product gas extraction opening 111 for exhausting the reaction product gas containing chlorosilane and a heater 112 for heating the reaction vessel are provided.

[Outer cylinder body]
The outer cylinder container main body 102 has a substantially cylindrical shape including a bottom plate (outer cylinder container bottom 103), and is made of metal such as aluminum, iron, and stainless steel.
Although a heat load of 1100 ° C. to 1400 ° C. is applied to the innermost brick layer by the heater 112 for heating the reaction vessel 105, the main body heat insulating layer 107 and the brick layer provided on the inner side of the outer tube container main body 102. Accordingly, the surface temperature of the outer cylinder container main body 102 becomes about 70 to 90 ° C.

The upper opening end of the outer cylinder container main body 102 is provided with a fastening means for attaching an outer cylinder container upper lid 104 described later. A fastening means will not be specifically limited if the inside of an outer cylinder container can be sealed airtightly.

In addition, a gas introduction opening 110 for supplying gas into the reaction vessel 105 is provided on the bottom plate of the outer cylinder vessel main body portion 102, and the reaction vessel 105 inner wall is provided on the side wall of the outer cylinder vessel main body portion 102. A reaction product gas extraction opening 111 is provided for exhausting the reaction product gas containing trichlorosilane produced in (1).

[Main body insulation layer]
A main body heat insulating layer 107 is provided inside the outer tube container main body 102 so as to cover it.
The main body heat insulating layer 107 is disposed so as not to transmit heat that could not be insulated by the brick layer 108 described later to the outside of the outer tube container main body portion 102. Therefore, the thermal load applied to the main body heat insulating layer 107 is It is small, about 800 ° C to 1200 ° C. Therefore, as a material constituting the main body heat insulating layer 107, the maximum use temperature may be low, but a material having more excellent heat insulating performance is preferable.

The main body heat insulating layer 107 is preferably composed of a plate-shaped heat insulating material. As such a heat insulating material, a heat insulating material mainly composed of alumina or silica can be cited, and the maximum use temperature is 1200 ° C. or higher. Some are preferably used.

For example, as a preferable heat insulating material, there can be mentioned a heat insulating board made of Khao wool (registered trademark) manufactured by Thermal Ceramics or Isowool (registered trademark) manufactured by Isolite Kogyo Co., Ltd.

[Brick layer]
A brick layer 108 formed by stacking a plurality of types of bricks having different properties is provided further inside the main body heat insulating layer 107. The brick layer 108 has a laminated structure in which an outermost brick layer, an intermediate brick layer, and an innermost brick layer are laminated in this order toward the center of the outer container body 102.

The brick layer 108 preferably has a two-layer structure in which each of the outermost brick layer (203 in FIG. 2) and the innermost brick layer (205 in FIG. 2) is one type. Or as shown in FIG. 2, it is good also as a 3 layer structure made into 1 type about each layer of the outermost brick layer 203, the intermediate | middle brick layer 204, and the innermost brick layer 205. As shown in FIG.
The number of layers constituting the brick layer is not particularly limited, and is appropriately set depending on the size of the reaction furnace and the reaction temperature.

The shape of the brick may be a substantially rectangular parallelepiped, or may be formed so as to have a slight curvature in accordance with the shape of the outer cylinder container main body that is substantially cylindrical.
Moreover, in order to laminate bricks, each member along the shape inside the side wall of the outer cylinder container main body 102 is used without using an adhesive or the like in order to avoid mixing the components in the adhesive into the reaction phase. Is preferably incorporated stably.

Also, each brick constituting the brick layer 108 is more preferably one that has been baked at 1800 ° C. to remove the binder and organic matter in order to avoid contamination by foreign matter in the reaction phase.

[Inner brick layer]
Since the innermost brick layer is disposed at a position closest to the reaction container among the heat insulating members of the outer cylinder container main body 102 and is exposed to a high temperature, a material having an excellent maximum use temperature is preferable.

The brick used for the innermost brick layer closest to the heater is subjected to a thermal load of about 1100 ° C to 1400 ° C, so the maximum operating temperature of the innermost brick layer is 1500 ° C or higher. Is preferred. Furthermore, it is preferable that the highest use temperature of the brick of an innermost brick layer is 1600 degreeC or more.

Further, since the innermost brick layer forms the inner wall surface of the outer cylinder container, it may come into contact with hydrogen, hydrogen chloride, or chlorosilanes leaked from the reaction container 105 and may be corroded by these substances. Therefore, it is preferably made of a material that does not react with these substances, has high erosion resistance to acidic and basic slugs, has high resistance to strong reducing gas such as H ₂ gas, and has chemical resistance.

The brick having such characteristics is preferably made of Al ₂ O ₃ , SiO ₂ , Fe ₂ O ₃ and having an Al ₂ O ₃ content of 99% or more.
Examples of such bricks include ISOLITE (registered trademark) BAL-99 manufactured by Isolite Industrial Co., Ltd., MB-G manufactured by AGC Ceramics Co., Ltd., and GM180H manufactured by Marukoshi Kogyo Co., Ltd.

[Outermost brick layer]
The outermost brick layer is disposed between the innermost brick layer and the main body heat insulating layer 107, and insulates heat that has not been insulated by the innermost brick layer.

Since the thermal load applied to the outermost brick layer is about 800 ° C. to 1200 ° C., the maximum use temperature may be lower than the brick of the innermost brick layer, but it is preferable to use one having excellent heat insulation performance.
As such a brick, it is preferable to use a low thermal conductivity brick having a thermal conductivity defined by JIS R 2616 of 0.7 W / m · K or less. Furthermore, it is preferable to use a low thermal conductivity brick having a thermal conductivity of 0.27 W / m · K or less.

The brick having such characteristics is preferably made of Al ₂ O ₃ , SiO ₂ , Fe ₂ O ₃ and having a content of Fe ₂ O ₃ of 1% or less.
Examples of such low thermal conductivity bricks include ISOLITE (registered trademark) LBK-28 manufactured by Isolite Industry Co., Ltd. and GM-13 manufactured by Marukoshi Industry Co., Ltd.

[Intermediate brick layer]
An intermediate brick layer may be provided between the innermost brick layer and the outermost brick layer.
The intermediate brick layer is disposed between the innermost brick layer and the outermost brick layer, and insulates heat that is not insulated by the innermost brick layer. The thermal load applied to the intermediate brick layer is about 1000 ° C to 1350 ° C.

The intermediate brick layer does not need to be resistant to these materials because it does not come into direct contact with hydrogen, hydrogen chloride, or chlorosilanes, but it uses bricks with better thermal insulation than the innermost brick layer. It is preferable.

Such a brick is preferably made of Al ₂ O ₃ , SiO ₂ , Fe ₂ O ₃ and having an Al ₂ O ₃ content of 90% or more.
Examples of such bricks include ISOLITE (registered trademark) BAL-90 manufactured by Isolite Kogyo Co., Ltd. and GM-160 manufactured by Marukoshi Kogyo Co., Ltd.

In the present embodiment, as shown in FIG. 1, the brick layer 108 is laminated at the bottom of the outer cylinder container main body 102 so as to surround the fixing plate 109 described later. If it can sufficiently withstand the weight of 105, the brick layer 108 can be laminated on the portion that contacts the fixing plate 109.

[Outer tube container top cover]
The outer cylinder container upper cover part 104 is a substantially disk-shaped member that hermetically seals the upper opening end of the outer cylinder container main body part 102 and is made of the same material as the outer cylinder container main body part 102.
The outer cylinder container upper cover part 104 is also provided with fastening means corresponding to the fastening means provided at the upper opening end of the outer cylinder container main body part 102. An upper lid heat insulating layer 106 is provided on the inner side of the outer cylinder container upper lid portion 104 so as not to leak the heat in the outer cylinder container main body portion 102 to the outside.

[Top cover insulation layer]
Since the upper lid heat insulating layer 106 constitutes the inner surface of the upper lid portion 104 of the outer cylinder container, the thermal load reaches about 1100 ° C. to 1400 ° C. like the innermost brick layer. Therefore, a material having excellent corrosion resistance against hydrogen, hydrogen chloride, and chlorosilanes that are excellent in the maximum use temperature and may leak from the reaction vessel 105 is preferable.

However, since the upper lid heat insulating layer 106 is attached to the inside of the outer cylinder container upper lid portion 104, it cannot be configured by incorporating bricks like the innermost brick layer. Therefore, it is preferable to use a material that has a high maximum use temperature, is excellent in corrosion resistance, and does not require incorporation, such as brick.
Examples of such a heat insulating material include a heat insulating material made of alumina fiber, such as Denka Arsene (registered trademark) manufactured by Denki Kagaku Kogyo Co., Ltd., and Isowool (registered trademark) manufactured by Isolite Industrial Co., Ltd. Can be mentioned.

Also, with respect to the terminal portion (not shown) of the heater 112 provided in the upper lid, the heat insulation efficiency can be improved by attaching a heat insulating material constituting the upper cover heat insulating layer. By setting it as such a structure, the heat leak from the terminal part of the heater 112 can be suppressed.

[Fixed plate]
As shown in FIG. 1, the bottom surface of the reaction vessel 105 is preferably installed on the outer cylinder vessel bottom 103 by a fixed plate 109.
The fixing plate 109 is arranged on the bottom plate (outer cylinder container bottom 103) of the outer cylinder container main body 102, receives and supports the total weight of the reaction container 105 described later, and fixes it. Therefore, it is necessary to use a member having excellent strength so as to withstand the weight of the reaction vessel 105 as a member constituting the fixing plate 109, and for example, graphite can be used.

The fixing plate 109 corresponds to the gas introduction opening 110 provided in the outer cylinder container main body 102 so that the gas supply into the reaction container 105 is not hindered when arranged on the bottom plate of the outer cylinder container main body 102. An opening is provided at a position to be used. The opening serves to fix the reaction vessel 105 by fitting a tubular projecting portion of a gas introduction opening 110 provided at the bottom of the reaction vessel 105 described later.

Furthermore, the fixed plate 109 has a plurality of holes penetrating in the thickness direction, that is, in the vertical direction when arranged between the bottom plate of the outer cylinder container main body 102 and the reaction vessel 105.

By providing a plurality of through holes in the fixing plate 109, an air layer is formed in the through hole portion. Since air has a lower thermal conductivity than materials such as graphite used for the fixed plate 109, the formation of an air layer by providing such a through hole suppresses the release of heat through the fixed plate 109. Insulation performance can be improved.
In addition, since the contact area between the fixed plate 109 and the reaction vessel can be reduced, heat transfer from the reaction vessel 105 to the fixed plate 109 can be prevented, and the heat insulation performance can be improved.

The number and shape of the holes provided in the fixing plate 109 are not particularly limited as long as sufficient strength can be secured to receive the total weight of the reaction vessel. Therefore, typically, as shown in FIG. 3, an opening for inserting the gas introduction opening 110 of the reaction vessel is provided at the center thereof, and a disk-like member having a plurality of through holes around the opening is provided. can do.

Further, it is preferable that a pedestal made of expanded graphite is further provided between the fixed plate 109 and the outer cylinder container main body 102 to further suppress heat transfer from the lower portion of the fixed plate 109 to the outer cylinder container main body 102.

[Reaction vessel]
The reaction vessel 105 is a substantially cylindrical vessel for reacting tetrachlorosilane and hydrogen in a high temperature environment. The reaction vessel 105 includes a gas introduction opening 110 for taking in tetrachlorosilane as a raw material and hydrogen gas, and a reaction product gas extraction opening 111 for deriving a reaction product gas containing trichlorosilane and hydrogen chloride. Have.
The gas introduction opening 110 has a configuration in which the periphery of the opening extends vertically from the bottom to form a tubular protrusion, and is fitted into the opening provided in the center of the fixing plate.
In this embodiment, as shown in FIG. 1, the gas introduction opening 110 is provided in the center of the bottom of the reaction furnace, and the reaction product gas extraction opening 111 is provided in the upper side wall of the reaction vessel 105. These positions are not limited to this.

[heater]
A plurality of heaters 112 are installed at a predetermined interval between the reaction vessel 105 and the outer cylinder vessel main body 102. In the present embodiment, the heater 112 is installed so as to be suspended from the outer cylinder container upper lid 104. However, the heater installation method is not limited to the hanging type, and for example, the outer cylinder container main body with the electrode on the lower side. You may install so that it may stand up from the bottom of a part.

Hereinafter, the effect of the reactor according to the present embodiment will be described.
According to the reactor according to the present embodiment, the inner side of the main body of the outer cylinder container includes a main body heat insulating layer and a brick layer, and the brick layer has a plurality of types of brick layers having different properties, that is, low thermal conductivity. Since it has the laminated structure laminated | stacked in order of the outermost brick layer and the high heat resistant innermost brick layer, heat insulation can be improved remarkably compared with the case where it consists only of a single heat insulating material.

Further, the thermal conductivity of the brick of the outermost brick layer is 0.7 W / m · K or less, and further the thermal conductivity of the brick of the outermost brick layer is 0.27 W / m · K or less, the reactor The heat insulation performance can be improved.

In addition, because the maximum use temperature of the innermost brick layer is 1500 ° C or higher, and the highest use temperature of the innermost brick layer brick is 1600 ° C or higher, it can be used for thermal loads reaching 1100 ° C to 1400 ° C. I can bear it. And the heat insulation and durability of a reaction furnace can be improved by using what was excellent in the corrosion resistance with respect to hydrogen, hydrogen chloride, and chlorosilanes for an innermost brick layer.

Also, by providing an intermediate brick layer between the outermost brick layer and the innermost brick layer, the heat insulation performance can be further improved.

And it is preferable to have further the fixing plate which has a some hole penetrated to the up-down direction which is arrange | positioned between the bottom plate of an outer cylinder container main-body part, and a reaction container, and supports a reaction container.
Thereby, the area which a reaction container and an outer cylinder container main-body part contact can be reduced, and it can prevent that heat transfers to the exterior. On the other hand, compared to the case where the weight of the reaction vessel is supported only by a tubular or columnar member, the reaction vessel is supported by a flat plate-like member, so that depending on the weight of the reaction vessel on the bottom of the reaction vessel or the member supporting the reaction vessel There is no local load.

Furthermore, since the reaction vessel is supported by depositing its entire weight on a fixed plate, it is not necessary to contact the upper cover of the outer tube vessel. Therefore, the area where the reaction container and the outer cylinder container come into contact can be reduced, and the heat of the reaction container can be prevented from escaping to the outside. In addition, since the reaction vessel is supported only by the fixed plate, even if the reaction vessel expands due to heating, distortion and breakage due to thermal expansion are unlikely to occur in the outer cylinder vessel main body and the reaction vessel.

Further, if the fixing plate is made of graphite, even if the number of holes is increased in order to improve the heat insulation performance, the graphite is excellent in strength, so that it has sufficient strength to support the reaction vessel. be able to.

In addition, when a pedestal made of expanded graphite is further provided between the fixed plate and the bottom plate of the outer cylinder container main body part, it is possible to suppress the movement of heat from the lower part of the fixed plate to the outer cylinder container main body part. It becomes possible.

Although the reaction furnace according to the present invention has been described above, the present invention is not limited to these.

[Example 1]
The reaction furnace as shown in FIG. 1 was produced using the outer cylinder container main body part which has the following heat insulation structures, and the reaction vessel fixing plate.
(Outer cylinder container top cover)
Alumina fiber (manufactured by Denki Kagaku Kogyo Co., Ltd .: Arsen (registered trademark)) was filled inside the outer lid portion of the outer cylinder container as an upper lid heat insulating layer.
(Outer cylinder body)
A heat insulation board (Iso wool (registered trademark) manufactured by Isolite Industry Co., Ltd.) was pasted as a main body heat insulation layer on the inner surface of the outer cylinder container main body, and the following heat-resistant bricks were stacked as a brick layer inside.
Inner brick layer: BAL-99
Outer brick layer: LBK-28
(Fixing plate)
As a fixed plate for supporting the reaction vessel, a graphite disc-like plate material having an opening for fitting the tubular projection of the gas inlet of the reaction vessel at the center and a plurality of through holes around it is used. It was.
The diameter of the through hole was 5% of the diameter of the fixed plate, and the through hole was formed so as to occupy an area of 30% of the fixed plate.

The outer cylinder container main body and the outer cylinder container upper lid were made of iron, and the reaction vessel was formed by connecting a plurality of substantially cylindrical carbon cylinders made of isotropic graphite whose surface was treated with a silicon carbide coating. A thing was used.

Using the reaction furnace, tetrachlorosilane and hydrogen (mole = 1: 1) source gas were reacted at normal pressure and reaction temperature of 1100 ° C.

At this time, the temperature of the surface part and outer peripheral surface part of the innermost brick layer of the reactor was measured. As a result, the temperature of the surface portion of the innermost brick layer was 1100 ° C., whereas the temperature of the outer peripheral surface portion was 150 ° C.
In addition, after continuously operating this reactor for 2000 hours, the apparatus was disassembled and the inside of the outer cylinder container main body, the brick layer, the fixed plate, etc. were observed, and any member was found to be distorted or damaged. There wasn't.

[Example 2]
In Example 2, the brick layer has a three-layer structure as shown in FIG.
At this time, BAL-90 was used for the intermediate brick layer. Other than that, the same experiment as in Example 1 was performed using a reactor manufactured in the same manner as in Example 1.

At this time, the temperature of the surface part and outer peripheral surface part of the innermost brick layer of the reactor was measured. As a result, the temperature of the surface portion of the innermost brick layer was 1100 ° C., whereas the temperature of the outer peripheral surface portion was 80 ° C.
When the apparatus was disassembled and the inside of the outer cylinder container main body, the brick layer, the fixing plate, and the like were observed, no distortion or breakage was observed in any of the members.

[Example 3]
In Example 3, a reactor similar to Example 2 was prepared except that a pedestal made of expanded graphite was disposed between the fixed plate and the outer cylinder container main body, and an experiment similar to Example 2 was performed. .

At this time, the temperatures of the bottom surface portion and the outer bottom surface portion of the innermost brick layer of the reactor were measured. As a result, the temperature of the bottom surface portion of the innermost brick layer of the reactor was 1100 ° C., whereas the temperature of the outer bottom surface portion was 80 ° C.
When the apparatus was disassembled and the inside of the outer cylinder container main body, the brick layer, the fixing plate, and the like were observed, no distortion or breakage was observed in any of the members.

In particular, it was confirmed that the temperature of the bottom surface of the main body of the outer cylinder container was 70% lower than that in Example 1, and the heat inside the reactor was hardly leaked to the outside.

[Comparative Example 1]
A single-layer brick layer was formed using only LBK-28.
And the reactor similar to Example 1 was produced, and the experiment similar to Example 1 was conducted.

At this time, the temperature of the surface part and outer peripheral surface part of the innermost brick layer of the reactor was measured. As a result, the temperature of the surface portion of the innermost brick layer was 1100 ° C., whereas the temperature of the outer peripheral surface portion was 250 ° C.
When the apparatus was disassembled and the inside of the outer cylinder container main body, the brick layer, the fixed plate, etc. were observed, the brick layer was corroded. Moreover, it was confirmed that the temperature of the outer peripheral surface of an outer cylinder container main-body part is clearly high compared with the case of Example 1, and the heat inside a reactor tends to leak outside.

<Discussion>
As can be seen from the above results, in the reactor of the example, even when the temperature inside the reaction vessel was operated to be 1100 ° C., the temperature of the outer cylinder vessel main body was 80 ° C. to 150 ° C. It turns out that it is excellent in.

Also, when the outer cylinder container main body is disassembled and examined, it is found that there is no distortion or breakage in the interior, and the durability is high.

Further, when the electric power applied to the heater was measured in order to bring the inside of the reaction furnace to the target temperature (about 1100 ° C.), it was reduced by 15% in the reaction furnace of the example with respect to the reaction furnace of the comparative example. Thus, it can be seen that the reaction furnace according to the present invention has high heat insulating properties, and thus has an effect of suppressing the manufacturing cost.

As shown in the above experimental results, the reactor according to the present invention has high heat insulation, can produce stable trichlorosilane, and is excellent in durability.

In the above, this invention was demonstrated based on the Example. However, those embodiments are merely examples of the present invention, and it will be understood by those skilled in the art that other various modifications are possible and that these modifications are also within the scope of the present invention.

Claims

A substantially cylindrical outer container body having a bottom plate;
An outer cylinder container upper lid for hermetically sealing the outer cylinder container main body,
A reaction vessel that is housed in the outer cylinder main body, a gas containing tetrachlorosilane and hydrogen is supplied to the inside, and a gas containing trichlorosilane and hydrogen chloride is generated;
An upper lid heat insulating layer covering the inner surface of the outer cylinder container upper lid portion;
A brick layer disposed on the inner surface of the outer container body,
A reactor having a laminated structure in which brick layers are laminated in order of an outermost brick layer having a low thermal conductivity and an innermost brick layer having a high heat resistance from the inner surface of the outer cylindrical container main body toward the center.
The reactor according to claim 1, wherein the bricks of the outermost brick layer have a thermal conductivity of 0.7 W / m · K or less.
The reactor according to claim 1, wherein the heat conductivity of the brick of the outermost brick layer is 0.27 W / m · K or less.
The reactor according to claim 1, wherein the highest use temperature of the brick of the innermost brick layer is 1500 ° C. or higher.
The reactor according to claim 1, wherein the highest use temperature of the brick of the innermost brick layer is 1600 ° C. or higher.
The reactor according to claim 1, wherein an intermediate brick layer is further provided between the outermost brick layer and the innermost brick layer.
2. The reaction according to claim 1, further comprising a fixing plate that is disposed between the bottom plate of the outer cylinder container main body and the reaction container and supports the reaction container and has a plurality of holes penetrating in the vertical direction. Furnace.
The reactor according to claim 5, wherein the fixed plate is made of graphite.
The reactor according to claim 5, further comprising a pedestal made of expanded graphite between the fixed plate and the bottom plate of the outer container body.