WO2010103631A1

WO2010103631A1 - Apparatus for producing trichlorosilane

Info

Publication number: WO2010103631A1
Application number: PCT/JP2009/054664
Authority: WO
Inventors: 靖史松尾; 晃一竹村
Original assignee: 電気化学工業株式会社
Priority date: 2009-03-11
Filing date: 2009-03-11
Publication date: 2010-09-16
Also published as: TW201036913A

Abstract

Disclosed is an apparatus having excellent heat resistance, which is used for producing trichlorosilane. The apparatus for producing trichlorosilane comprises a reactor (1) which is provided with a reaction chamber (10) wherein a reaction product gas containing trichlorosilane and hydrogen chloride is produced from a raw material gas containing tetrachlorosilane and hydrogen, a heater (11) for heating the reaction chamber (10), and an outer cylindrical case (12) for housing the reaction chamber (10) and the heater (11); a quenching tower (4) for cooling the reaction product gas; a connection cylinder (3) provided with a first bellows pipe (30) which expandably/contractibly connects the reactor (1) and the quenching tower (4); an extraction pipe (2) so arranged from the reaction chamber (10) to the quenching tower (4) passing through inside of the connection cylinder (3) as to guide the reaction product gas from the reactor (1) to the quenching tower (4); and a second bellows pipe (31) arranged substantially coaxially with the extraction pipe (2) within the connection cylinder (3) so as to cover the extraction pipe (2), while having one end joined to the inner circumferential surface of the connection cylinder (3) and the other end joined to the outer circumferential surface of the extraction pipe (2).

Description

トリクロロシラン製造装置Trichlorosilane production equipment

　本発明は、テトラクロロシランと水素とを反応させてトリクロロシランに転換する、耐熱性に優れたトリクロロシラン製造装置に関する。 The present invention relates to a trichlorosilane production apparatus excellent in heat resistance, in which tetrachlorosilane and hydrogen are reacted to convert to trichlorosilane.

　トリクロロシラン（ＳｉＨＣｌ_３）は、半導体、液晶パネル、太陽電池等の製造に用いられる特殊材料ガスである。近年、需要は順調に拡大し、エレクトロニクス分野で広く使用されるＣＶＤ材料として、今後も伸びが期待されている。 Trichlorosilane (SiHCl ₃ ) is a special material gas used for manufacturing semiconductors, liquid crystal panels, solar cells, and the like. In recent years, demand has been steadily expanding, and growth is expected as a CVD material widely used in the electronics field.

　トリクロロシランは、テトラクロロシラン（ＳｉＣｌ_４）と水素（Ｈ_２）とを接触させ、以下の熱平衡状態を達成することによって生成される。
ＳｉＣｌ_４＋Ｈ_２⇔ＳｉＨＣｌ_３＋ＨＣｌ　　　　　（１）
　この反応は、ガス化したテトラクロロシランと水素からなる原料ガスを反応容器において８００℃～１３００℃に加熱することによって行われる。 Trichlorosilane is produced by contacting tetrachlorosilane (SiCl ₄ ) and hydrogen (H ₂ ) to achieve the following thermal equilibrium state.
SiCl ₄ + H ₂ ⇔SiHCl ₃ + HCl (1)
This reaction is performed by heating a raw material gas composed of gasified tetrachlorosilane and hydrogen to 800 ° C. to 1300 ° C. in a reaction vessel.

　反応容器から排出される高温の反応生成ガスには、生成されたトリクロロシランおよび塩化水素の他、多量の未反応テトラクロロシランおよび水素が含まれている。反応生成ガスからトリクロロシランを取り出すには、テトラクロロシランとトリクロロシランの沸点の相違を利用して蒸留塔で凝縮する方法が用いられる。具体的には、コンデンサーにおいて、凝縮分であるクロロシランと、未凝縮分である塩化水素、水素、未凝縮クロロシランとに分け、さらに、深冷分離により－７０℃程度まで冷却して凝縮分からトリクロロシランを分離する。 The high temperature reaction product gas discharged from the reaction vessel contains a large amount of unreacted tetrachlorosilane and hydrogen in addition to the generated trichlorosilane and hydrogen chloride. In order to extract trichlorosilane from the reaction product gas, a method of condensing in a distillation column using the difference in boiling point between tetrachlorosilane and trichlorosilane is used. Specifically, in the condenser, it is divided into a chlorosilane that is a condensed component and hydrogen chloride, hydrogen, and an uncondensed chlorosilane that is an uncondensed component, and further cooled to about −70 ° C. by deep-cooling separation, and then trichlorosilane from the condensed component Isolate.

　反応生成ガスから目的とするトリクロロシランを分離するにあたり、反応容器から導出されたばかりの高温の反応生成ガスをいきなり蒸留塔に導入してしまうと蒸留塔に過度の負荷がかかるため、典型的には、反応生成ガスを蒸留塔に導入する前に急冷塔において予備的に冷却しておく必要がある。 When separating the target trichlorosilane from the reaction product gas, if the high-temperature reaction product gas just introduced from the reaction vessel is suddenly introduced into the distillation column, an excessive load is applied to the distillation column. Before the reaction product gas is introduced into the distillation tower, it is necessary to preliminarily cool it in the quenching tower.

　しかし、予備的冷却とはいっても、冷却力が不十分であると平衡がテトラクロロシラン側に傾き、一旦は生成したトリクロロシランが再びテトラクロロシランへと戻ってしまう。そこで、トリクロロシランの回収効率の向上を図るために、平衡が十分にトリクロロシラン側に達した時点で反応生成ガスを可能な限り瞬時に所定温度まで冷却して平衡を凍結する必要がある。上記平衡状態を瞬時に凍結するには、典型的には、反応生成ガスを１秒未満のうちに６００℃程度にまで急冷する必要がある。 However, even if it is preliminary cooling, if the cooling power is insufficient, the equilibrium is inclined to the tetrachlorosilane side, and once generated trichlorosilane returns to tetrachlorosilane again. Therefore, in order to improve the recovery efficiency of trichlorosilane, it is necessary to cool the reaction product gas to a predetermined temperature as quickly as possible when the equilibrium sufficiently reaches the trichlorosilane side and freeze the equilibrium. In order to instantly freeze the equilibrium state, it is typically necessary to rapidly cool the reaction product gas to about 600 ° C. in less than one second.

　テトラクロロシランと水素とを反応させてトリクロロシランに転換し、さらに反応生成ガスを冷却する機構を備えた反応容器としては、例えば特許文献１に記載されたものがある。この文献には、テトラクロロシランと水素を反応室に導入して６００℃～１２００℃の温度で転換反応させることによってトリクロロシランと塩化水素とを含む反応生成ガスを得た後、反応室から導出された反応生成ガスに室温に冷却されたクロロシラン混合物を噴霧により接触させ、１秒以内に３００℃以下にまで急冷する冷却手段を備えた装置が提案されている。 As a reaction vessel equipped with a mechanism for reacting tetrachlorosilane with hydrogen to convert to trichlorosilane and further cooling the reaction product gas, there is one described in Patent Document 1, for example. In this document, a reaction product gas containing trichlorosilane and hydrogen chloride is obtained by introducing tetrachlorosilane and hydrogen into a reaction chamber and performing a conversion reaction at a temperature of 600 ° C. to 1200 ° C., and then derived from the reaction chamber. There has been proposed an apparatus provided with a cooling means for bringing the chlorosilane mixture cooled to room temperature into contact with the reaction product gas by spraying and rapidly cooling to 300 ° C. or less within 1 second.

　また、特許文献２には、温度１２００℃をこえ１４００℃以下に加熱した反応器にＳｉＣｌ_４とＨ_２とのモル比が１：１～１：２の混合ガスを導入して反応させ熱平衡状態とし（その平衡状態の混合物であるＳｉＣｌ_４とＨ_２とのモル比が１：１～１：４）、さらにＳｉＨＣｌ_３とＨＣｌ等を含有する混合物を１秒以内に６００℃以下に急冷して反応を凍結させることによりＳｉＨＣｌ_３の収率及び収量を向上させるＳｉＨＣｌ_３の製造法が記載されている。 In Patent Document 2, a gas mixture having a molar ratio of SiCl ₄ and H ₂ of 1: 1 to 1: 2 is introduced into a reactor heated to a temperature of 1200 ° C. over 1200 ° C. and reacted to cause a thermal equilibrium state. (Molar ratio of SiCl ₄ and H _{2 in} the equilibrium mixture is 1: 1 to 1: 4), and the mixture containing SiHCl ₃ and HCl is rapidly cooled to 600 ° C. or less within 1 second. A process for producing SiHCl ₃ is described that improves the yield and yield of SiHCl ₃ by freezing the reaction.

特公昭５７－３８５２４公報Japanese Patent Publication No.57-38524 特開昭６０－８１０１０号公報JP 60-81010 A

発明の概要Summary of the Invention

　ところで、特許文献１に記載の装置では、反応炉と急冷塔とが急冷塔の側方に設けられた接続管を介して接続されており、接続管と反応炉との接合部には閉じた端部が形成されている。この閉じた端部にゾンデを貫通させ、当該ゾンデを介して反応炉で生成した反応ガスを急冷室へと導出している。 By the way, in the apparatus described in Patent Document 1, the reaction furnace and the quenching tower are connected via a connection pipe provided on the side of the quenching tower, and the connection between the connection pipe and the reaction furnace is closed. An end is formed. A sound is passed through the closed end, and the reaction gas generated in the reaction furnace is led to the quenching chamber through the sound.

　しかし、高温に達している反応炉と低温の急冷室とは、接続管と反応炉との接合部における閉じた端部壁面によって遮られているため、急冷塔と反応炉とを遮る端部壁面とその近傍には局所的に大きな温度差が生じる。その結果、当該部位に熱膨張による応力が集中し、歪みや破損を生じる場合がある。また、端部壁面に貫通して固定されているゾンデが熱膨張しても、ゾンデと端部壁面との接合部に応力が集中し、歪みや破損に至る場合がある。 However, the reactor wall that reaches the high temperature and the low-temperature quenching chamber are blocked by the closed end wall at the junction between the connecting pipe and the reactor, and therefore the end wall that blocks the quenching tower and the reactor. There is a large temperature difference locally in the vicinity of it. As a result, stress due to thermal expansion concentrates on the part, which may cause distortion or breakage. Moreover, even if the sound that penetrates and is fixed to the end wall surface is thermally expanded, stress may be concentrated on the joint between the sound and the end wall surface, resulting in distortion or breakage.

　また、特許文献２に記載の装置では、反応器の排気側端部に反応生成ガスを導出するための取り出し管、例えば毛細管やラパール管が挿入されており、取り出し管と反応器の排気側端部との接合部は、反応生成ガスが漏れないように気密に固定されている。反応生成ガスは、この取り出し管を通過する際に自然に冷却される。 Moreover, in the apparatus described in Patent Document 2, a take-out pipe for leading out reaction product gas, for example, a capillary tube or a lapar pipe, is inserted into the exhaust side end of the reactor, and the take-out pipe and the exhaust side end of the reactor The joint with the part is airtightly fixed so that the reaction product gas does not leak. The reaction product gas is naturally cooled as it passes through the take-out pipe.

　ところが、上記構成の装置では、反応生成ガスの冷却が取り出し管を通過する際の自然冷却に任されているため、必ずしも冷却速度および冷却能力の点で十分とは言えない。また、反応器の排気側端部やそれに貫通して固定されている取り出し管が熱膨張すると、これらの接合部に応力が加わり、歪みや破損を生じる場合がある。 However, in the apparatus having the above-described configuration, cooling of the reaction product gas is left to natural cooling when passing through the take-out pipe, so that it cannot always be said that the cooling rate and the cooling capacity are sufficient. Further, when the exhaust side end portion of the reactor or the take-out pipe fixed through it is thermally expanded, stress is applied to these joint portions, which may cause distortion or breakage.

　本発明は上記事情に鑑みてなされたものであり、反応炉と急冷塔との連結部に熱膨張による歪みや破損を生じないことが可能なトリクロロシラン製造装置を提供することを目的とする。より具体的には、高温条件で反応ガスを生成する反応炉と反応ガスを冷却する急冷塔とを繋ぐ連結筒、連結筒内において反応炉と急冷塔との間の空間を遮断する遮断部材、並びに、反応炉に収容されている反応容器から反応生成ガスを前記連結筒内を通して急冷塔へと導出する抜出管において、熱膨張により発生する応力を吸収するとともに、当該熱膨張による応力の発生を低減するトリクロロシラン製造装置を提供することを目的とする。 The present invention has been made in view of the above circumstances, and an object thereof is to provide an apparatus for producing trichlorosilane capable of preventing distortion and breakage due to thermal expansion at a connecting portion between a reaction furnace and a quenching tower. More specifically, a connecting cylinder that connects a reaction furnace that generates a reaction gas under a high temperature condition and a quenching tower that cools the reaction gas, a blocking member that blocks a space between the reaction furnace and the quenching tower in the connection cylinder, In addition, in the extraction pipe for leading the reaction product gas from the reaction vessel accommodated in the reaction furnace to the quenching tower through the inside of the connecting cylinder, the stress generated by the thermal expansion is absorbed and the stress is generated by the thermal expansion. An object of the present invention is to provide an apparatus for producing trichlorosilane that reduces the above-described problem.

　本発明は、前記課題を解決するために以下の構成を採用した。すなわち、本発明のトリクロロシラン製造装置は、
　テトラクロロシランと水素とを含む原料ガスからトリクロロシランと塩化水素とを含む反応生成ガスを生成する反応容器と、前記反応容器を加熱するヒータと、前記反応容器およびヒータを収容する外筒容器とを備える反応炉と、
　前記反応生成ガスを冷却する急冷塔と、
　前記反応炉と急冷塔との間を伸縮可能に連結する第一ベローズ管を備えた連結筒と、
　前記反応容器から前記連結筒内部を通って前記急冷塔に至るように配され、前記反応生成ガスを反応炉から急冷塔に導出する抜出管と、
　前記連結筒内部において前記抜出管を覆うように略同軸に配され、一端が連結筒の内周に接合され、他端が抜出管の外周に接合された第二ベローズ管と
を備えていることを特徴とする。 The present invention employs the following configuration in order to solve the above problems. That is, the trichlorosilane production apparatus of the present invention is
A reaction vessel for producing a reaction product gas containing trichlorosilane and hydrogen chloride from a raw material gas containing tetrachlorosilane and hydrogen, a heater for heating the reaction vessel, and an outer cylinder vessel for housing the reaction vessel and the heater. A reactor equipped with,
A quenching tower for cooling the reaction product gas;
A connecting cylinder including a first bellows pipe that connects the reaction furnace and the quenching tower in an extendable manner;
An extraction pipe arranged from the reaction vessel to the quenching tower through the inside of the connecting cylinder, and leading the reaction product gas from the reaction furnace to the quenching tower;
A second bellows pipe disposed substantially coaxially so as to cover the extraction pipe inside the connection cylinder, one end joined to the inner periphery of the connection cylinder, and the other end joined to the outer periphery of the extraction pipe. It is characterized by being.

　このトリクロロシラン製造装置では、反応炉と急冷塔とを連結する連結筒が蛇腹構造を有する第一ベローズ管を備えていることにより、連結筒に熱が加わった際に熱膨張により生じる応力を第一ベローズ管の形状が変化することで吸収することができる。そのため、連結筒の熱膨張による破損を防ぐことができ、装置の安定性、安全性を高めることができる。 In this trichlorosilane manufacturing apparatus, the connecting cylinder connecting the reactor and the quenching tower includes the first bellows pipe having the bellows structure, so that stress generated by thermal expansion when heat is applied to the connecting cylinder is reduced. Absorption can be achieved by changing the shape of one bellows tube. Therefore, damage due to thermal expansion of the connecting cylinder can be prevented, and the stability and safety of the apparatus can be improved.

　さらに、反応炉内部の空間と急冷塔内部の空間とが、抜出管と連結筒との間にこれらとほぼ同軸に配された第二ベローズ管によって遮断されているため、抜出管が熱膨張しても、遮断手段である第二ベローズ管がこれに追随して適宜伸縮して、これを吸収することができる。そのため、熱膨張によって抜出管や遮断手段が破損することを防ぐことができ、装置の安定性、安全性を高めることができるとともに、両塔間の気密状態をより安定に維持することができる。 Furthermore, since the space inside the reactor and the space inside the quenching tower are blocked by the second bellows pipe disposed almost coaxially between the extraction pipe and the connecting cylinder, the extraction pipe is heated. Even if it expand | swells, the 2nd bellows pipe | tube which is a interruption | blocking means can follow this, can be expanded-contracted suitably, and can absorb this. Therefore, it is possible to prevent the extraction tube and the shut-off means from being damaged due to thermal expansion, to improve the stability and safety of the apparatus, and to maintain the airtight state between both towers more stably. .

　また、反応炉と急冷塔との連結部に二重にベローズ管を配設したことにより、熱膨張以外の原因により発生した応力も吸収できる。そのため、例えば、耐震性においても優れている。 In addition, the double bellows tube provided at the connection between the reaction furnace and the quenching tower can absorb stress generated due to causes other than thermal expansion. Therefore, for example, it is excellent also in earthquake resistance.

　さらに、高温の外筒容器内の空間と低温の急冷塔内の空間とが第二ベローズ管により遮断されているため、当該第二ベローズ管の内外で熱交換が行われる。本発明では、第二ベローズ管が連結筒内部において抜出管を覆うようにこれと略同軸に配されていることから、第二ベローズ管に沿って外筒容器側から急冷塔側にかけて温度が緩やかに下降する中間的な温度帯域を形成することができる。その結果、抜出管にかかる熱的負荷を当該帯域にわたって広く分散でき、抜出管に局所的に大きな応力が発生することを防止することができる。 Furthermore, since the space in the high temperature outer cylinder container and the space in the low temperature quenching tower are blocked by the second bellows pipe, heat exchange is performed inside and outside the second bellows pipe. In the present invention, since the second bellows pipe is arranged substantially coaxially so as to cover the extraction pipe inside the connecting cylinder, the temperature is increased from the outer cylinder container side to the quenching tower side along the second bellows pipe. An intermediate temperature zone that gradually falls can be formed. As a result, the thermal load applied to the extraction pipe can be widely distributed over the band, and a large stress can be prevented from being locally generated in the extraction pipe.

　本発明に係るトリクロロシラン製造装置によれば、反応炉と急冷塔とを連結する連結筒が第一ベローズ管を備え、かつ、連結筒内において反応炉と急冷塔とが抜出管とほぼ同軸に配された第二ベローズ管によって遮断されているため、これらの部位における熱膨張による破損を防ぐことができ、装置の安定性、安全性を高めることができる。 According to the trichlorosilane production apparatus according to the present invention, the connecting cylinder connecting the reaction furnace and the quenching tower includes the first bellows pipe, and the reaction furnace and the quenching tower are substantially coaxial with the extraction pipe in the connecting cylinder. Since it is interrupted | blocked by the 2nd bellows pipe | tube arrange | positioned by these, the damage by thermal expansion in these parts can be prevented, and stability and safety | security of an apparatus can be improved.

　そして、さらに特筆すべきことに、本発明に係るトリクロロシラン製造装置によれば、連結筒内部において抜出管を覆うように第二ベローズ管を配したことにより、連結筒内部に中間的な温度帯域が形成され抜出管にかかる熱的負荷を分散できるため、抜出管に局所的に大きな応力が生じることを防止することができる。 And, more particularly, according to the trichlorosilane manufacturing apparatus according to the present invention, by arranging the second bellows pipe so as to cover the extraction pipe inside the connection cylinder, an intermediate temperature is provided inside the connection cylinder. Since a zone is formed and the thermal load applied to the extraction pipe can be dispersed, it is possible to prevent a large stress from being locally generated in the extraction pipe.

本発明の実施形態であるトリクロロシラン製造装置の説明図である。It is explanatory drawing of the trichlorosilane manufacturing apparatus which is embodiment of this invention. 本発明の実施形態であるトリクロロシラン製造装置の連結筒周辺の概略縦断面図である。It is a schematic longitudinal cross-sectional view of the connection cylinder periphery of the trichlorosilane manufacturing apparatus which is embodiment of this invention.

符号の説明Explanation of symbols

１：反応炉
２：抜出管
３：連結筒
４：急冷塔
１０：反応容器
１１：ヒータ
１２：外筒容器
１３：原料ガス導入口
１４：反応生成ガス抜出口
１５：発熱体
１６：電極
１７：原料ガス導入開口部
１８：反応生成ガス抜出開口部
２１：第一部材
２２：第二部材
２３：第三部材
２４：反応生成ガス吹き出し部
２５：突出部
３０：第一ベローズ管
３１：第二ベローズ管
３２：第一筒状部材
３３：第二筒状部材
３４：収容部
３５：直立部
３６：拡径部
３７：縁部
３８：鍔部
３９：板材
４０：金属製容器
４１：スプレーノズル
４２：ポンプ
４３：冷却装置
４４：導管
４５：反応生成ガス導入開口部 1: Reaction furnace 2: Extraction pipe 3: Connecting cylinder 4: Rapid cooling tower 10: Reaction vessel 11: Heater 12: Outer cylinder vessel 13: Raw material gas inlet 14: Reaction product gas outlet 15: Heating element 16: Electrode 17 : Source gas introduction opening 18: Reaction product gas extraction opening 21: First member 22: Second member 23: Third member 24: Reaction product gas blowout part 25: Protrusion part 30: First bellows pipe 31: First Double bellows tube 32: first tubular member 33: second tubular member 34: accommodating portion 35: upright portion 36: diameter-expanding portion 37: edge portion 38: flange portion 39: plate material 40: metal container 41: spray nozzle 42: Pump 43: Cooling device 44: Conduit 45: Reaction product gas introduction opening

発明を実施するための形態BEST MODE FOR CARRYING OUT THE INVENTION

　以下、本発明の実施の形態について、図面を用いて説明する。尚、すべての図面において、同様な構成要素には同一の符号を付し、適宜説明を省略する。 Hereinafter, embodiments of the present invention will be described with reference to the drawings. In all the drawings, the same components are denoted by the same reference numerals, and description thereof will be omitted as appropriate.

　図１は、本発明に係るトリクロロシラン製造装置の一実施形態を概略的に示したものである。また、図２は当該トリクロロシラン製造装置の連結筒周辺の断面を概略的に示したものである。 FIG. 1 schematically shows an embodiment of a trichlorosilane production apparatus according to the present invention. FIG. 2 schematically shows a cross section around the connecting cylinder of the trichlorosilane production apparatus.

　本実施形態のトリクロロシラン製造装置は、図１および図２に示すように、
テトラクロロシランと水素とを含む原料ガスからトリクロロシランと塩化水素とを含む反応生成ガスを生成する反応容器１０と、前記反応容器１０を加熱するヒータ１１と、前記反応容器１０およびヒータ１１を収容する外筒容器１２とを備える反応炉１と、
　前記反応生成ガスを冷却する急冷塔４と、
　前記反応炉１と急冷塔４との間を伸縮可能に連結する第一ベローズ管３０を備えた連結筒３と、
　前記反応容器１０から前記連結筒３内部を通って前記急冷塔４に至るように配され、前記反応生成ガスを反応炉１から急冷塔４に導出する抜出管２と、
　前記連結筒３内部において前記抜出管２を覆うように略同軸に配され、一端が連結筒３の内周に接合され、他端が抜出管２の外周に接合された第二ベローズ管３１と
を備えている。 As shown in FIG. 1 and FIG. 2, the trichlorosilane production apparatus of this embodiment is
A reaction vessel 10 for generating a reaction product gas containing trichlorosilane and hydrogen chloride from a raw material gas containing tetrachlorosilane and hydrogen, a heater 11 for heating the reaction vessel 10, and the reaction vessel 10 and the heater 11 are accommodated. A reactor 1 comprising an outer tube container 12;
A quenching tower 4 for cooling the reaction product gas;
A connecting cylinder 3 having a first bellows pipe 30 that connects the reaction furnace 1 and the quenching tower 4 in an extendable manner;
An extraction pipe 2 that is arranged so as to reach the quenching tower 4 from the reaction vessel 10 through the inside of the connecting cylinder 3, and leads the reaction product gas from the reaction furnace 1 to the quenching tower 4;
A second bellows pipe disposed substantially coaxially so as to cover the extraction pipe 2 inside the connection cylinder 3, one end joined to the inner periphery of the connection cylinder 3, and the other end joined to the outer periphery of the extraction pipe 2. 31.

＜反応炉＞
　反応炉１は、反応容器１０と、当該反応容器１０の外側を囲むように配される長尺のヒータ１１と、前記反応容器１０およびヒータ１１を収容する外筒容器１２とを備える。ヒータ１１で反応容器１０の外壁を加熱することにより、反応容器１０の底部に設けられた原料ガス導入口１３から供給されるテトラクロロシランと水素との混合ガスを反応容器１０内部において約８００℃から約１３００℃の高温で反応させ、トリクロロシランと塩化水素を含む反応生成ガスを生成する。 <Reactor>
The reaction furnace 1 includes a reaction vessel 10, a long heater 11 disposed so as to surround the outside of the reaction vessel 10, and the outer vessel 12 that accommodates the reaction vessel 10 and the heater 11. By heating the outer wall of the reaction vessel 10 with the heater 11, the mixed gas of tetrachlorosilane and hydrogen supplied from the raw material gas inlet 13 provided at the bottom of the reaction vessel 10 is about 800 ° C. inside the reaction vessel 10. The reaction is performed at a high temperature of about 1300 ° C. to produce a reaction product gas containing trichlorosilane and hydrogen chloride.

＜反応容器＞
　反応容器１０は、テトラクロロシランと水素とを高温環境下で反応させるための略円筒形状の容器であり、原料ガスを取り込むための原料ガス導入口１３と、反応生成ガスを導出するための反応生成ガス抜出口１４とを有する。本実施形態では、原料ガス導入口１３を反応容器１０の底部中央に設け、反応生成ガス抜出口１４を反応容器１０の上方の側壁に設ける構成としているが、これらの設置位置はこれに限定されるものではない。 <Reaction vessel>
The reaction vessel 10 is a substantially cylindrical vessel for reacting tetrachlorosilane and hydrogen in a high temperature environment, a raw material gas inlet 13 for taking in a raw material gas, and a reaction product for deriving a reaction product gas. And a gas outlet 14. In the present embodiment, the raw material gas inlet 13 is provided in the center of the bottom of the reaction vessel 10 and the reaction product gas outlet 14 is provided on the upper side wall of the reaction vessel 10, but these installation positions are limited to this. It is not something.

　反応容器１０を構成する材質は、気密性に優れた黒鉛材であり、特に、微粒子構造のため強度が高く、熱膨張等の特性がどの方向に対しても同一であることから耐熱性および耐食性にも優れている等方性高純度黒鉛を用いることが好ましい。 The material constituting the reaction vessel 10 is a graphite material having excellent airtightness, and particularly has high strength due to the fine particle structure, and the characteristics such as thermal expansion are the same in any direction, so that it has heat resistance and corrosion resistance. It is preferable to use isotropic high-purity graphite, which is also excellent.

　特に、反応容器１０の内周面および／または外周面が炭化ケイ素被膜処理されていること、当該炭化ケイ素被膜がＣＶＤ法により１０～５００μｍの厚みで形成されていることが好ましい。炭化ケイ素被膜は化学的分解に対して極めて高い耐性を有するため、カーボン組織の化学的浸食を防止できる。そのため、炭化ケイ素被膜処理を施すことにより、反応容器１０の表面を腐食から保護することができる。 In particular, it is preferable that the inner peripheral surface and / or the outer peripheral surface of the reaction vessel 10 is treated with a silicon carbide coating, and the silicon carbide coating is formed with a thickness of 10 to 500 μm by a CVD method. Since the silicon carbide coating has a very high resistance to chemical degradation, chemical erosion of the carbon structure can be prevented. Therefore, the surface of the reaction vessel 10 can be protected from corrosion by performing the silicon carbide coating treatment.

＜ヒータ＞
　ヒータ１１は、上下方向に延びる複数の長尺のカーボン製発熱体１５と、当該発熱体１５の一端に接続され発熱体１５に電力を供給するための電極１６とを備える。ヒータ１１は、反応容器１０の周囲を複数で取り囲むように配され、供給電力量を制御することにより反応容器１０内部の温度を反応容器１０の外側から調節する。 <Heater>
The heater 11 includes a plurality of elongated carbon heating elements 15 extending in the vertical direction and an electrode 16 connected to one end of the heating element 15 for supplying power to the heating element 15. The heater 11 is arranged so as to surround the reaction vessel 10 in a plurality, and controls the temperature inside the reaction vessel 10 from the outside of the reaction vessel 10 by controlling the amount of power supplied.

＜外筒容器＞
　外筒容器１２は、外側がステンレス等の金属からなり、内側がカーボンボード、耐火レンガ、断熱レンガ等の断熱材で被覆された略円筒形状の容器である。外筒容器１２は、前記反応容器１０および前記ヒータ１１を収容し、これらを外界から断熱する。外筒容器１２には、反応容器１０を収容した際に、その原料ガス導入口１３および反応生成ガス抜出口１４に対応する位置にそれぞれ原料ガス導入開口部１７および反応生成ガス抜出開口部１８が設けられている。反応生成ガス抜出開口部１８にはフランジ等の継手手段が設けられており、後述する連結筒３と接続可能とされている。 <Outer cylinder container>
The outer cylinder container 12 is a substantially cylindrical container whose outer side is made of a metal such as stainless steel and whose inner side is covered with a heat insulating material such as a carbon board, a refractory brick, or a heat insulating brick. The outer cylinder container 12 accommodates the reaction container 10 and the heater 11 and insulates them from the outside. When the reaction vessel 10 is accommodated in the outer cylinder vessel 12, the source gas introduction opening 17 and the reaction product gas extraction opening 18 are respectively located at positions corresponding to the source gas introduction port 13 and the reaction product gas extraction port 14. Is provided. The reaction product gas extraction opening 18 is provided with joint means such as a flange, and can be connected to a connecting cylinder 3 described later.

＜連結筒＞
　本実施形態の連結筒３は、
　一端に反応炉１の反応生成ガス抜出開口部１８に接続される継手手段を有し他端に拡径された収容部３４を有する第一筒状部材３２と、
　一端に前記第一筒状部材３２の収容部３４側に挿入される挿入側端部を有し他端に急冷塔４に接続される継手手段を有する第二筒状部材３３と、
　前記収容部３４に収容され一端が第一筒状部材３２の収容部３４側端部に固定され他端が第二筒状部材３３の挿入側端部に固定される第一ベローズ管３０と
を備えている。 <Connecting cylinder>
The connecting cylinder 3 of this embodiment is
A first cylindrical member 32 having a coupling means connected to the reaction product gas extraction opening 18 of the reaction furnace 1 at one end and an accommodating portion 34 having an enlarged diameter at the other end;
A second tubular member 33 having an insertion side end inserted into the accommodating portion 34 side of the first tubular member 32 at one end and joint means connected to the quenching tower 4 at the other end;
A first bellows pipe 30 that is housed in the housing portion 34 and has one end fixed to the end portion on the housing portion 34 side of the first cylindrical member 32 and the other end fixed to the insertion side end portion of the second tubular member 33. I have.

＜第一筒状部材＞
　第一筒状部材３２は、ステンレスなどの金属からなり、一端に外筒容器１２の反応生成ガス抜出開口部１８に接続可能なフランジ等の継手手段を有し、他端に第一ベローズ管３０を収容するための収容部３４を有する。収容部３４は、第一筒状部材３２の径方向外側に垂直に延伸する直立部３５と、当該直立部３５から軸方向に沿って延伸する拡径部３６と、当該拡径部３６から径方向内側に垂直に延伸する縁部３７とからなる。 <First cylindrical member>
The first cylindrical member 32 is made of a metal such as stainless steel, and has a joint means such as a flange that can be connected to the reaction product gas extraction opening 18 of the outer cylinder container 12 at one end, and a first bellows pipe at the other end. A housing portion 34 for housing 30 is provided. The accommodating portion 34 includes an upright portion 35 that extends perpendicularly outward in the radial direction of the first cylindrical member 32, a diameter-expanded portion 36 that extends from the upright portion 35 along the axial direction, and a diameter from the diameter-expanded portion 36. It consists of the edge part 37 extended | stretched perpendicularly | vertically to a direction inner side.

　前記縁部３７は第一ベローズ管３０の一端を固定する部位であり、縁部３７の径方向内側への突出幅は、第一ベローズ管３０の一端を固定できる限りにおいて、第二筒状部材３３の挿入を妨げず、しかも挿入された第二筒状部材３３が軸方向および径方向に自由に動くことを妨げない範囲とされる。 The edge portion 37 is a portion for fixing one end of the first bellows tube 30, and the projecting width inward in the radial direction of the edge portion 37 is the second cylindrical member as long as one end of the first bellows tube 30 can be fixed. It is set as a range that does not prevent the insertion of 33 and does not prevent the inserted second cylindrical member 33 from freely moving in the axial direction and the radial direction.

＜第二筒状部材＞
　第二筒状部材３３は、前記第一筒状部材３２と同様にステンレスなどの金属からなり、一端に後述する急冷塔４の反応生成ガス導入開口部４５に接続するためのフランジ等の継手手段を有し、他端（前記第一筒状部材３２の収容部３４側に挿入される挿入側端部）に第二筒状部材３３の径方向外側に垂直に延伸する鍔部３８を有する。 <Second cylindrical member>
The second cylindrical member 33 is made of a metal such as stainless steel like the first cylindrical member 32, and has a joint means such as a flange for connecting to a reaction product gas introduction opening 45 of the quenching tower 4 to be described later at one end. The other end (the insertion side end inserted into the accommodating portion 34 side of the first cylindrical member 32) has a flange portion 38 extending perpendicularly to the radially outer side of the second cylindrical member 33.

　前記鍔部３８は第一ベローズ管３０の一端を固定する部位であり、鍔部３８の径方向外側への突出幅は、第一ベローズ管３０の一端を固定できる限りにおいて、第一筒状部材３２への挿入を妨げず、しかも第一筒状部材３２に挿入された状態で第二筒状部材３３が軸方向および径方向に自由に動くことを妨げない範囲とされる。 The flange portion 38 is a portion for fixing one end of the first bellows tube 30, and the protruding width of the flange portion 38 to the outer side in the radial direction is the first cylindrical member as long as one end of the first bellows tube 30 can be fixed. The second cylindrical member 33 is in a range that does not prevent the second cylindrical member 33 from freely moving in the axial direction and the radial direction while being inserted into the first cylindrical member 32.

＜第一ベローズ管＞
　第一ベローズ管３０は、金属から構成された筒状の蛇腹構造を備えた部材であり、軸心方向に伸縮可能であるとともに、径方向にも変形可能となっている。この第一ベローズ管３０は金属製であればよいが、ステンレス鋼製であればより好適でありオーステナイト系ステンレス鋼製でもフェライト系ステンレス鋼製でもよい。 <First bellows tube>
The first bellows tube 30 is a member having a cylindrical bellows structure made of metal, and can be expanded and contracted in the axial direction and can also be deformed in the radial direction. The first bellows tube 30 may be made of metal, but is more preferably made of stainless steel, and may be made of austenitic stainless steel or ferritic stainless steel.

　第一ベローズ管３０は、山の高さが入口径の２～１０％程度、山と山との間隔が全長の２～８％程度であるものが好ましい。さらに、軸と垂直方向の変位量が第一ベローズ管３０の入口径の３～１０％、軸方向の変位量が全長の２～５％程度であるものが好ましい。また、山の間隔や高さは均一であっても不均一であってもよい。 The first bellows tube 30 preferably has a peak height of about 2 to 10% of the inlet diameter and a distance between the peaks of about 2 to 8% of the total length. Further, it is preferable that the amount of displacement in the direction perpendicular to the axis is 3 to 10% of the inlet diameter of the first bellows tube 30, and the amount of displacement in the axial direction is about 2 to 5% of the total length. Further, the intervals and heights of the peaks may be uniform or non-uniform.

　上記構成の連結筒３では、第一ベローズ管３０は、第一筒状部材３２の収容部３４に格納され、その両端が第一筒状部材３２の縁部３７および第二筒状部材３３の鍔部３８の対向面にそれぞれ固定された構成とされる。従って、第一ベローズ管３０はその内側が第二筒状部材３３の胴体部によって覆われることになる。 In the connecting cylinder 3 configured as described above, the first bellows tube 30 is stored in the accommodating portion 34 of the first cylindrical member 32, and both ends thereof are the edges 37 of the first cylindrical member 32 and the second cylindrical member 33. It is set as the structure fixed to the opposing surface of the collar part 38, respectively. Therefore, the inside of the first bellows tube 30 is covered with the body portion of the second cylindrical member 33.

　上記構成の連結筒３を組み立てるには、例えば、第一ベローズ管３０の両端を第一筒状部材３２の縁部３７および第二筒状部材３３の鍔部３８にそれぞれ固定し、その状態で第二筒状部材３３を第一筒状部材３２に挿入して第一ベローズ管３０を収容部３４に格納してもよい。また、第一筒状部材３２の縁部３７に相当する部材を別途取り付ける構成としてもよい。 To assemble the connecting cylinder 3 having the above-described configuration, for example, both ends of the first bellows pipe 30 are fixed to the edge portion 37 of the first cylindrical member 32 and the flange portion 38 of the second cylindrical member 33, respectively. The first bellows tube 30 may be stored in the accommodating portion 34 by inserting the second cylindrical member 33 into the first cylindrical member 32. Moreover, it is good also as a structure which attaches the member corresponded to the edge part 37 of the 1st cylindrical member 32 separately.

＜急冷塔＞
　急冷塔４は、円筒状の金属製容器４０と、当該容器内に設置され容器内に冷却液を噴霧するスプレーノズル４１と、前記容器の底に溜まった冷却液を取り出してスプレーノズル４１に循環させるポンプ４２と、冷却液を冷却するための冷却装置４３と、急冷塔４の頂部から冷却後の反応生成ガスを取り出すための導管４４とを備える。急冷塔４の側壁には前記連結筒３を接続するための反応生成ガス導入開口部４５が設けられており、当該反応生成ガス導入開口部４５には連結筒３と接続するためのフランジ等の継手手段が設けられている。スプレーノズル４１は、急冷塔４に導入される反応生成ガスに向けて冷却液を噴霧できるよう、反応生成ガス導入開口部４５の上部近傍に設置される。 <Quenching tower>
The quenching tower 4 includes a cylindrical metal container 40, a spray nozzle 41 that is installed in the container and sprays the coolant in the container, and the coolant accumulated in the bottom of the container is taken out and circulated to the spray nozzle 41. A cooling pump 43 for cooling the coolant, and a conduit 44 for taking out the reaction product gas after cooling from the top of the quenching tower 4. A reaction product gas introduction opening 45 for connecting the connecting cylinder 3 is provided on the side wall of the quenching tower 4. The reaction product gas introduction opening 45 has a flange or the like for connecting to the connection cylinder 3. Joint means are provided. The spray nozzle 41 is installed in the vicinity of the upper portion of the reaction product gas introduction opening 45 so that the coolant can be sprayed toward the reaction product gas introduced into the quenching tower 4.

　冷却液は、トリクロロシランとテトラクロロシランとの混合液で構成され、テトラクロロシランとトリクロロシランの全体量に対するテトラクロロシランの比は、１～０．５である。温度は、６０℃以下とすることが好ましい。例えば、テトラクロロシラン：トリクロロシランの組成比が８５：１５、温度が４０℃程度のものを好適に使用することができる。 The cooling liquid is composed of a mixed liquid of trichlorosilane and tetrachlorosilane, and the ratio of tetrachlorosilane to the total amount of tetrachlorosilane and trichlorosilane is 1 to 0.5. The temperature is preferably 60 ° C. or lower. For example, a tetrachlorosilane: trichlorosilane composition ratio of 85:15 and a temperature of about 40 ° C. can be preferably used.

　急冷塔４の頂部から取り出された冷却後の反応生成ガスは、導管４４を経てさらに蒸留塔（不図示）へと送られ、目的とするトリクロロシランの分離が行われる。 The cooled reaction product gas taken out from the top of the quenching tower 4 is further sent to a distillation tower (not shown) through a conduit 44, and the intended trichlorosilane is separated.

＜抜出管＞
　抜出管２は、連結筒３内部を通って反応容器１０内部と急冷塔４内部とを繋ぐカーボン製の管状部材であり、反応容器１０内の反応生成ガスを急冷塔４に導出する。 <Extraction pipe>
The extraction pipe 2 is a carbon tubular member that connects the inside of the reaction vessel 10 and the inside of the quenching tower 4 through the inside of the connecting cylinder 3, and guides the reaction product gas in the reaction vessel 10 to the quenching tower 4.

　抜出管２を構成する材質は、気密性に優れた黒鉛材であり、特に、微粒子構造のため強度が高く、熱膨張等の特性がどの方向に対しても同一であることから耐熱性および耐食性にも優れている等方性高純度黒鉛を用いることが好ましい。 The material constituting the extraction pipe 2 is a graphite material having excellent airtightness, and particularly has high strength due to the fine particle structure, and has the same characteristics such as thermal expansion in any direction. It is preferable to use isotropic high-purity graphite that is also excellent in corrosion resistance.

　特に、抜出管２の内周面および／または外周面が炭化ケイ素被膜処理されていること、当該炭化ケイ素被膜がＣＶＤ法により１０～５００μｍの厚みで形成されていることが好ましい。炭化ケイ素被膜は化学的分解に対して極めて高い耐性を有するため、カーボン組織の化学的浸食を防止できる。そのため、炭化ケイ素被膜処理を施すことにより、抜出管２の表面を腐食から保護することができる。 In particular, it is preferable that the inner peripheral surface and / or the outer peripheral surface of the extraction pipe 2 is treated with a silicon carbide coating, and that the silicon carbide coating is formed with a thickness of 10 to 500 μm by a CVD method. Since the silicon carbide coating has a very high resistance to chemical degradation, chemical erosion of the carbon structure can be prevented. Therefore, the surface of the extraction pipe 2 can be protected from corrosion by performing the silicon carbide coating treatment.

　抜出管２は、気密性や強度の点で優れることから単一の部材からなるものが好ましいが、複数の部材を連結したものであってもよい。本実施形態の抜出管２は、複数の部材から構成され、装置を組み立てた際に、主に反応炉１内に位置する第一部材２１、主に連結筒３内に位置する第二部材２２、および主に冷却塔内に位置する第三部材２３とからなる。すなわち、第一部材２１は、一端に反応容器１０の反応生成ガス抜出口１４との接続部を有し他端に第二部材２２を連結するための継手手段を有し、第二部材２２は、両端に第一部材２１または第三部材２３を連結するための継手手段を有し、第三部材２３は、一端に第二部材２２を連結するための継手手段を有し他端に反応生成ガス吹き出し部２４を有する。 The extraction tube 2 is preferably made of a single member because it is excellent in terms of airtightness and strength, but it may be formed by connecting a plurality of members. The extraction pipe 2 of the present embodiment is composed of a plurality of members, and when the apparatus is assembled, the first member 21 mainly located in the reaction furnace 1 and the second member mainly located in the connecting cylinder 3. 22 and a third member 23 mainly located in the cooling tower. That is, the first member 21 has a connecting portion with one end of the reaction product gas outlet 14 of the reaction vessel 10 at one end and a joint means for connecting the second member 22 at the other end. The joint member for connecting the first member 21 or the third member 23 is connected to both ends, and the third member 23 has the joint means for connecting the second member 22 to one end, and the reaction is generated at the other end. A gas blowing part 24 is provided.

　抜出管２の継手手段は、後述する第二ベローズ管３１が接合されるように抜出管２の外周側に突出部２５を形成するものとされる。このような突出部２５を形成する継手手段としては、典型的には、フランジを用いることができる。また、略円筒状の管状部材を用い、突き合わせ端部を外側からリングで螺合締結するものでもよい。この場合には、リングが第二ベローズ管３１を固定するための突出部２５を形成する。 The joint means of the extraction pipe 2 is such that a protruding portion 25 is formed on the outer peripheral side of the extraction pipe 2 so that a second bellows pipe 31 described later is joined. As a joint means for forming such a protrusion 25, a flange can be typically used. Alternatively, a substantially cylindrical tubular member may be used and the butted end portion may be screwed and fastened from the outside with a ring. In this case, the ring forms a protrusion 25 for fixing the second bellows pipe 31.

＜第二ベローズ管＞
　第二ベローズ管３１は、金属から構成された蛇腹構造の部材であり、軸心方向に伸縮可能であるとともに、径方向にも変形可能となっている。第一ベローズ管３０と同様に、この第二ベローズ管３１は金属製であればよいが、ステンレス鋼製であればより好適でありオーステナイト系ステンレス鋼製でもフェライト系ステンレス鋼製でもよい。また、単層であっても多層であってもよいが、多層構造の場合は耐腐食性が増すため好ましい。 <Second bellows tube>
The second bellows tube 31 is a member having a bellows structure made of metal, and can be expanded and contracted in the axial direction and can also be deformed in the radial direction. Similar to the first bellows pipe 30, the second bellows pipe 31 may be made of metal, but is more preferably made of stainless steel, and may be made of austenitic stainless steel or ferritic stainless steel. Moreover, although it may be a single layer or a multilayer, a multilayer structure is preferable because corrosion resistance is increased.

　第二ベローズ管３１は、山の高さが入口径の２～１０％程度、山と山との間隔が全長の２～８％程度であるものが好ましい。さらに、軸と垂直方向の変位量が第二ベローズ管３１の入口径の３～１０％、軸方向の変位量が全長の２～５％程度であるものが好ましい。また、山の間隔や高さは均一であっても不均一であってもよい。 The second bellows pipe 31 preferably has a peak height of about 2 to 10% of the inlet diameter and a distance between the peaks of about 2 to 8% of the total length. Further, it is preferable that the amount of displacement in the direction perpendicular to the axis is 3 to 10% of the inlet diameter of the second bellows pipe 31, and the amount of displacement in the axial direction is about 2 to 5% of the total length. Further, the intervals and heights of the peaks may be uniform or non-uniform.

　第二ベローズ管３１は、連結筒３内部において抜出管２の外側にこれを覆うようにほぼ同軸で配され、一端が連結筒３の内周に接合され、他端が抜出管２の外周に接合される。
　本実施形態では、第二ベローズ管３１と連結筒３内周との接続は、外筒容器１２の反応生成ガス抜出開口部１８に設けられた継手手段と連結筒３の第一筒状部材３２に設けられた継手手段との間にドーナツ状の板材３９を挟み込み、当該板材３９の連結筒３内に張り出した部分に第二ベローズ管３１の一端を固定することによって行われる。また、第二ベローズ管３１と抜出管２外周との接続は、抜出管２を構成する第二部材２２と第三部材２３との連結部に形成された突出部２５に第二ベローズ管３１の一端を固定することによって行われる。
このようにして、反応炉１内部の空間と急冷塔４内部の空間とが連結筒３内に配置された第二ベローズ管３１によって遮断される。 The second bellows pipe 31 is arranged substantially coaxially so as to cover the outside of the extraction pipe 2 inside the connection cylinder 3, one end is joined to the inner periphery of the connection cylinder 3, and the other end is the extraction pipe 2. Joined to the outer periphery.
In the present embodiment, the connection between the second bellows pipe 31 and the inner periphery of the connecting cylinder 3 is performed by the joint means provided in the reaction product gas extraction opening 18 of the outer cylinder container 12 and the first cylindrical member of the connecting cylinder 3. The doughnut-shaped plate member 39 is sandwiched between the joint means provided at 32 and one end of the second bellows pipe 31 is fixed to a portion of the plate member 39 protruding into the connecting tube 3. In addition, the connection between the second bellows pipe 31 and the outer periphery of the extraction pipe 2 is such that the second bellows pipe is connected to the projecting portion 25 formed at the connecting portion between the second member 22 and the third member 23 constituting the extraction pipe 2. This is done by fixing one end of 31.
In this way, the space inside the reaction furnace 1 and the space inside the quenching tower 4 are blocked by the second bellows pipe 31 arranged in the connecting cylinder 3.

　本実施形態では、連結筒３を構成する部材を伸縮自在な第一ベローズ管３０で接続しているため、連結筒３に局所的に大きな温度差がかかって第一筒状部材３２および第二筒状部材３３が熱膨張したとしても、第一ベローズ管３０の形状が変化することで連結筒３に係る応力を吸収することができ、連結筒３の歪みや破損を回避することができる。 In the present embodiment, since the members constituting the connecting cylinder 3 are connected by the first bellows pipe 30 which can be expanded and contracted, a large temperature difference is locally applied to the connecting cylinder 3 and the first cylindrical member 32 and the second cylindrical member 32. Even if the cylindrical member 33 is thermally expanded, the stress relating to the connecting cylinder 3 can be absorbed by the shape of the first bellows tube 30 being changed, and the distortion or breakage of the connecting cylinder 3 can be avoided.

　また、第一ベローズ管３０の外側が第一筒状部材３２の拡径部３６で覆われ、内側が第二筒状部材３３の胴体部によって覆われるため、連結筒３内部に存在し得る化学物質、すなわち反応生成ガスや冷却液中に含まれる反応性物質が第一ベローズ管３０に付着してこれを劣化し伸縮性を損ねることを防止できる。 Further, since the outer side of the first bellows tube 30 is covered with the enlarged diameter portion 36 of the first cylindrical member 32 and the inner side is covered with the body portion of the second cylindrical member 33, chemicals that may exist inside the connecting cylinder 3. It is possible to prevent a substance, that is, a reactive substance contained in the reaction product gas or the cooling liquid from adhering to the first bellows pipe 30 and deteriorating it, thereby impairing the stretchability.

　また、連結筒３内周と抜出管２外周との間に接続され反応炉１内部の空間と急冷塔４内部の空間とを遮断する手段として、伸縮可能な第二ベローズ管３１を用いることにより、抜出管２が熱膨張または収縮しても、これに追従して第二ベローズ管３１が適宜伸縮するため、抜出管２を破損することがなく、両空間の遮断状態が破られることもない。 In addition, a second bellows pipe 31 that can be expanded and contracted is used as a means that is connected between the inner periphery of the connecting cylinder 3 and the outer periphery of the extraction pipe 2 to block the space inside the reactor 1 and the space inside the quenching tower 4. Therefore, even if the extraction pipe 2 is thermally expanded or contracted, the second bellows pipe 31 is appropriately expanded and contracted following this, so that the extraction pipe 2 is not damaged and the shut-off state of both spaces is broken. There is nothing.

そしてさらに、第二ベローズ管３１が連結筒３内部において抜出管２を覆うようにこれと略同軸に配されていることから、第二ベローズ管３１に沿って外筒容器１２側から急冷塔４側にかけて温度が緩やかに下降する中間的な温度帯域を形成することができる。その結果、抜出管２にかかる熱的負荷を当該帯域にわたって広く分散でき、抜出管２に局所的に大きな応力が発生することを防止することができる。 Further, since the second bellows pipe 31 is arranged substantially coaxially with the extraction pipe 2 so as to cover the extraction pipe 2 inside the connecting cylinder 3, the quenching tower from the outer cylinder container 12 side along the second bellows pipe 31. An intermediate temperature zone can be formed in which the temperature gradually decreases toward the side 4. As a result, the thermal load applied to the extraction pipe 2 can be widely distributed over the band, and it is possible to prevent a large stress from being locally generated in the extraction pipe 2.

　なお、本発明の技術範囲は上記実施形態に限定されるものではなく、本発明の趣旨を逸脱しない範囲において種々の変更を加えることが可能である。 The technical scope of the present invention is not limited to the above embodiment, and various modifications can be made without departing from the spirit of the present invention.

　例えば、反応容器は、優れた耐久性や伝熱効率を実現するために本来は一体成型されていることが好ましいが、製造技術上の問題から、略円筒体を複数連結一体化させたものが用いられる。略円筒体を複数連結一体化させる反応容器としては、特に、複数の略円筒体を、端部同士を突き合わせて略同軸に上下に配し、突き合わせ端部を外側からリングで螺合締結するものが好ましい。このような構造とすることにより、略円筒体の構造を単純なものとすることができ、上端または下端に肉厚の薄い部位が形成されないため、物理的衝撃に対して優れた耐性を有する。また、連結部において一方の略円筒体の端部が他方の略円筒体の端部に嵌合するような構成ではないため、高温環境下で使用することにより略円筒体が熱膨張しても、個々の略円筒体の熱膨張係数の相違による連結部の割れやひび割れを引き起こすことがない。そのため、反応容器の構成部材を交換する頻度が低減され、装置の作業能率を改善することができる。 For example, it is preferable that the reaction vessel is originally integrally molded in order to achieve excellent durability and heat transfer efficiency. However, due to problems in manufacturing technology, a reaction vessel in which a plurality of substantially cylindrical bodies are connected and integrated is used. It is done. As a reaction vessel for connecting and integrating a plurality of substantially cylindrical bodies, in particular, a plurality of substantially cylindrical bodies are arranged substantially vertically on the same end, but end to end with each other, and the abutting ends are screwed and fastened from the outside with a ring. Is preferred. By adopting such a structure, the structure of the substantially cylindrical body can be simplified, and since a thin portion is not formed at the upper end or the lower end, it has excellent resistance to physical impact. In addition, since the end portion of one substantially cylindrical body is not fitted to the end portion of the other substantially cylindrical body in the connecting portion, even if the substantially cylindrical body is thermally expanded by using it in a high temperature environment. In addition, there is no possibility of causing cracks or cracks in the connecting portion due to the difference in thermal expansion coefficient between individual substantially cylindrical bodies. Therefore, the frequency of exchanging the components of the reaction vessel is reduced, and the working efficiency of the apparatus can be improved.

　また、上記実施態様では、第一ベローズ管が第一筒状部材の収容部に格納され、その内側が第二筒状部材の胴体部によって覆われるように構成したが、第一筒状部材と第二筒状部材との連結部に第一ベローズ管が用いられていれば連結筒にかかる応力を十分に吸収することができるため、第一ベローズ管が第一筒状部材と第二筒状部材との間に収容されていなくても構わない。 Moreover, in the said embodiment, although the 1st bellows pipe was stored in the accommodating part of the 1st cylindrical member, and the inside was covered with the trunk | drum part of the 2nd cylindrical member, If the first bellows tube is used in the connecting portion with the second cylindrical member, the stress applied to the connecting tube can be sufficiently absorbed, so that the first bellows tube is the first cylindrical member and the second cylindrical member. It does not need to be accommodated between the members.

　また、上記実施態様では、第二ベローズ管の反応炉側端部を連結筒に接続し、急冷塔側端部を抜出管に接続するように構成したが、これを逆に接続しても構わない。すなわち、第二ベローズ管と連結筒内側との接続を、外筒容器の急冷塔の反応生成ガス導入開口部に設けられた継手手段と連結筒の第二筒状部材に設けられた継手手段との間にドーナツ状の板材を挟み込み、当該板材の連結筒内に張り出した部分に第二ベローズ管の一端を固定することによって行い、第二ベローズ管と抜出管外側との接続を、抜出管を構成する第一部材と第二部材との連結部に形成された突出部に第二ベローズ管の一端を固定することによって行ってもよい。 In the above embodiment, the reactor side end of the second bellows pipe is connected to the connecting cylinder, and the quench tower side end is connected to the extraction pipe. I do not care. That is, the connection between the second bellows pipe and the inner side of the connecting cylinder is made by using a joint means provided at the reaction product gas introduction opening of the quenching tower of the outer cylinder container and a joint means provided at the second cylindrical member of the connecting cylinder; The doughnut-shaped plate material is sandwiched between the two, and one end of the second bellows tube is fixed to the portion of the plate material that protrudes into the connecting tube, and the connection between the second bellows tube and the outside of the extraction tube is extracted. You may perform by fixing the end of a 2nd bellows pipe | tube to the protrusion part formed in the connection part of the 1st member and 2nd member which comprise a pipe | tube.

　さらに、上記実施態様では、抜出管が３つの部材から構成されているが、単一の部材からなるものであっても、あるいはさらに多くの部材から構成されるものであってもよい。 Furthermore, in the above embodiment, the extraction pipe is composed of three members, but it may be composed of a single member or a larger number of members.

　以下、本発明を実施例によりさらに説明するが、本発明はこれらに限定されるものではない。 Hereinafter, the present invention will be further described with reference to examples, but the present invention is not limited thereto.

実施例１
　図２に示すトリクロロシラン製造装置を使用してトリクロロシランの製造を行い、連結筒、抜出管、および第二ベローズ管における歪みや破損の有無を調べた。 Example 1
Trichlorosilane was manufactured using the trichlorosilane manufacturing apparatus shown in FIG. 2, and the presence or absence of distortion or breakage in the connecting tube, the extraction tube, and the second bellows tube was examined.

＜装置説明＞
　この装置には以下の部材を用いた。 <Device description>
The following members were used for this apparatus.

連結筒：
　ステンレス製の筒状部材をステンレス鋼製のベローズ管（厚み：２ｍｍ）を介して連結した連結筒を用いた。このベローズ管の軸と垂直方向の変位量が入口径の５％程度、軸方向の変位量が全長の５％程度であった。 Connecting cylinder:
A connecting cylinder in which stainless steel cylindrical members were connected via a stainless steel bellows tube (thickness: 2 mm) was used. The amount of displacement in the direction perpendicular to the axis of the bellows tube was about 5% of the inlet diameter, and the amount of displacement in the axial direction was about 5% of the total length.

第二ベローズ管：
ステンレス鋼製のベローズ管を用いた。このベローズ管の軸と垂直方向の変位量が入口径の５％程度、軸方向の変位量が全長の５％程度であった。 Second bellows tube:
A stainless steel bellows tube was used. The amount of displacement in the direction perpendicular to the axis of the bellows tube was about 5% of the inlet diameter, and the amount of displacement in the axial direction was about 5% of the total length.

抜出管：
炭化ケイ素被膜処理を施したカーボン製の管状部材を用いた。 Extraction pipe:
A carbon tubular member subjected to a silicon carbide coating treatment was used.

＜実験条件＞
　上記の装置を用いて、反応炉においてテトラクロロシランと水素（モル＝１：１）の原料ガスを、常圧、反応温度１１００℃にて反応させ、反応生成ガスを抜出管を介して急冷塔に取り出し、２０℃に温度調節した冷却液（トリクロロシラン濃度２０％）を用いて冷却した。 <Experimental conditions>
Using the above apparatus, the reaction gas of tetrachlorosilane and hydrogen (mole = 1: 1) is reacted at normal pressure at a reaction temperature of 1100 ° C. in the reaction furnace, and the reaction product gas is quenched through an extraction pipe. And cooled using a cooling liquid whose temperature was adjusted to 20 ° C. (trichlorosilane concentration 20%).

　このトリクロロシラン製造装置を連続的に２０００時間運転した後、装置を解体して連結筒、抜出管、および第二ベローズ管を観察したところ、いずれの部材にも歪みや破損は観察されなかった。 After this trichlorosilane production apparatus was continuously operated for 2000 hours, the apparatus was disassembled and the connecting cylinder, the extraction pipe, and the second bellows pipe were observed, and no distortion or breakage was observed in any of the members. .

比較例１
　第二ベローズ管の代わりに蛇腹構造を有しない筒状部材（厚み：２ｍｍ）を配設したこと以外は、上記実施例１と同様にトリクロロシラン製造装置を整えた。この筒状部材は、実施例１で使用した第二ベローズ管と同じ材質からなる。 Comparative Example 1
A trichlorosilane production apparatus was prepared in the same manner as in Example 1 except that a cylindrical member (thickness: 2 mm) having no bellows structure was disposed instead of the second bellows pipe. This cylindrical member is made of the same material as the second bellows pipe used in the first embodiment.

　このトリクロロシラン製造装置を、実施例１と同様に運転し、装置を解体して連結筒、抜出管、および筒状部材を観察したところ、抜出管と筒状部材とに歪みが認められた。 When this trichlorosilane production apparatus was operated in the same manner as in Example 1, the apparatus was disassembled, and the connecting cylinder, the extraction pipe, and the cylindrical member were observed. As a result, distortion was observed in the extraction pipe and the cylindrical member. It was.

比較例２
　第二ベローズ管の代わりに、抜出管が貫通可能な開口を有する板状部材（厚み：２ｍｍ）を用いて反応炉側の空間と急冷塔側の空間とを連結筒の中央付近で遮断したこと以外は、上記実施例１と同様にトリクロロシラン製造装置を整えた。この筒状部材は、実施例１で使用した第二ベローズ管と同じ材質からなる。 Comparative Example 2
Instead of the second bellows pipe, a plate-like member (thickness: 2 mm) having an opening through which the extraction pipe can penetrate was used to block the space on the reactor side and the space on the quenching tower near the center of the connecting cylinder. A trichlorosilane production apparatus was prepared in the same manner as in Example 1 except that. This cylindrical member is made of the same material as the second bellows pipe used in the first embodiment.

　このトリクロロシラン製造装置を、実施例１と同様に運転し、装置を解体して連結筒、抜出管、および板状部材を観察したところ、板状部材と接合した部位において抜出管に歪みが認められた。 When this trichlorosilane production apparatus was operated in the same manner as in Example 1, the apparatus was disassembled and the connecting cylinder, the extraction pipe, and the plate member were observed, and the extraction pipe was distorted at the portion joined to the plate member. Was recognized.

比較例３
　連結筒の代わりに、第一ベローズ管を有しない筒状部材（厚み：２ｍｍ）を配設したこと以外は、上記実施例１と同様にトリクロロシラン製造装置を整えた。この筒状部材は、実施例１で使用した連結筒の第一および第二筒状部材と同じ材質からなる。 Comparative Example 3
A trichlorosilane production apparatus was prepared in the same manner as in Example 1 except that a cylindrical member (thickness: 2 mm) having no first bellows pipe was disposed instead of the connecting cylinder. This cylindrical member consists of the same material as the 1st and 2nd cylindrical member of the connection cylinder used in Example 1. FIG.

　このトリクロロシラン製造装置を、実施例１と同様に運転し、装置を解体して筒状部材、抜出管、および第二ベローズ管を観察したところ、筒状部材に歪みが認められた。 When this trichlorosilane production apparatus was operated in the same manner as in Example 1, the apparatus was disassembled, and the cylindrical member, the extraction tube, and the second bellows tube were observed. As a result, distortion was observed in the cylindrical member.

　＜実験の考察＞
　以上の比較実験から明らかなように、反応炉と急冷塔とを連結する連結筒が第一ベローズ管を備え、かつ、反応炉と急冷塔とが抜出管と連結筒との間に配された第二ベローズ管によって遮断される構成とすることにより、熱膨張によるこれらの部材の歪みや破損を防ぐことができ、装置の安定性、安全性を高めることができた。また、連結筒内部において抜出管を覆うように第二ベローズ管を配したことにより、抜出管にかかる熱的負荷を分散でき、抜出管に局所的に大きな応力が生じることを防止することができた。 <Experimental considerations>
As is clear from the above comparative experiment, the connecting cylinder connecting the reaction furnace and the quenching tower includes the first bellows pipe, and the reaction furnace and the quenching tower are arranged between the extraction pipe and the connecting cylinder. By adopting a configuration that is blocked by the second bellows pipe, it was possible to prevent distortion and breakage of these members due to thermal expansion, and to improve the stability and safety of the apparatus. Moreover, by arranging the second bellows pipe so as to cover the extraction pipe inside the connecting cylinder, the thermal load applied to the extraction pipe can be dispersed, and a large stress is prevented from being locally generated in the extraction pipe. I was able to.

　以上、本発明を実施例に基づいて説明した。この実施例はあくまで例示であり、種々の変形例が可能なこと、またそうした変形例も本発明の範囲にあることは当業者に理解されるところである。 In the above, this invention was demonstrated based on the Example. It is to be understood by those skilled in the art that this embodiment is merely an example, and that various modifications are possible and that such modifications are within the scope of the present invention.

Claims

　テトラクロロシランと水素とを含む原料ガスからトリクロロシランと塩化水素とを含む反応生成ガスを生成する反応容器と、反応容器を加熱するヒータと、反応容器およびヒータを収容する外筒容器とを備える反応炉と、
　反応生成ガスを冷却する急冷塔と、
　反応炉と急冷塔との間を伸縮可能に連結する第一ベローズ管を備えた連結筒と、
　反応容器から連結筒内部を通って急冷塔に至るように配され、反応生成ガスを反応炉から急冷塔に導出する抜出管と、
　連結筒内部において抜出管を覆うように略同軸に配され、一端が連結筒の内周に接合され、他端が抜出管の外周に接合された第二ベローズ管と
を備えるトリクロロシラン製造装置。 Reaction comprising: a reaction vessel that generates a reaction product gas containing trichlorosilane and hydrogen chloride from a raw material gas containing tetrachlorosilane and hydrogen; a heater that heats the reaction vessel; and a reaction vessel and an outer cylinder that houses the heater A furnace,
A quenching tower for cooling the reaction product gas;
A connecting cylinder having a first bellows pipe that connects the reaction furnace and the quenching tower in an extendable manner;
An extraction pipe arranged from the reaction vessel to the quenching tower through the inside of the connecting cylinder, and leading the reaction product gas from the reaction furnace to the quenching tower;
Trichlorosilane manufacturing provided with a second bellows pipe arranged substantially coaxially so as to cover the extraction pipe inside the connection cylinder, one end joined to the inner periphery of the connection cylinder and the other end joined to the outer periphery of the extraction pipe apparatus.
　連結筒が、
　一端に反応炉に接続される継手手段を有し他端に拡径された収容部を有する第一筒状部材と、
　一端に第一筒状部材の収容部側に挿入される挿入側端部を有し他端に急冷塔に接続される継手手段を有する第二筒状部材と、
　収容部に収容され一端が第一筒状部材の収容部側端部に固定され他端が第二筒状部材の挿入側端部に固定される第一ベローズ管と
を備える請求項１記載のトリクロロシラン製造装置。 The connecting cylinder
A first tubular member having a joint means connected to the reaction furnace at one end and an accommodating portion having an enlarged diameter at the other end;
A second cylindrical member having an insertion side end inserted into the accommodating portion side of the first cylindrical member at one end and joint means connected to the quenching tower at the other end;
The first bellows tube, which is housed in the housing portion, has one end fixed to the housing portion side end portion of the first cylindrical member, and the other end fixed to the insertion side end portion of the second tubular member. Trichlorosilane production equipment.
第一ベローズ管の軸と垂直方向の変位量が入口径の３～１０％であり、軸方向の変位量が全長の２～５％である請求項１記載のトリクロロシラン製造装置。 The trichlorosilane production apparatus according to claim 1, wherein the displacement of the first bellows pipe in the direction perpendicular to the axis is 3 to 10% of the inlet diameter, and the displacement in the axial direction is 2 to 5% of the total length.
　第二ベローズ管の軸と垂直方向の変位量が入口径の３～１０％であり、軸方向の変位量が全長の２～５％である請求項１記載のトリクロロシラン製造装置。 The apparatus for producing trichlorosilane according to claim 1, wherein the displacement of the second bellows pipe in the direction perpendicular to the axis is 3 to 10% of the inlet diameter, and the amount of displacement in the axial direction is 2 to 5% of the total length.