JP2014227322A - Manufacturing apparatus and manufacturing method of monosilane - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a manufacturing apparatus and a manufacturing method of a monosilane capable of realizing a high monosilane yield by using a minimal raw ingredient without entailing a yield loss attributed to an excessive reaction and of continuously preparing a monosilane having a high stability.SOLUTION: The provided apparatus includes: a reaction column 1 for preparing a monosilane by using a hydrogenated silicon chloride as a raw ingredient and a tertiary aliphatic hydrocarbon-substituted amine and/or the hydrochloride of a tertiary aliphatic hydrocarbon-substituted amine as a catalyst; a separator 2 in which a monosilane is extracted from a reaction product supplied from the upper stage 1c of the reaction column 1 and separated from a condensate liquid consisting of other components; an evaporation tank 3 in which a concentrated liquid is prepared by heating a bottom liquid supplied from the lower stage 1b of the reaction column 1 and then evaporating the hydrogenated silicon chloride included within the bottom liquid; and a catalyst regeneration tank 5 in which a mixture obtained by adding a portion of the raw ingredient and/or a portion of the condensate liquid to the concentrated liquid is heated so as to reactivate the catalyst included within the condensate liquid and to prepare a regenerant including the catalyst. A circulatory system targeting the catalyst is formed by the supply, into the reaction column 1, of the regenerant supplied from the catalyst regeneration tank 5.

Description

  The present invention relates to a monosilane production apparatus and method, and more specifically, to a monosilane production apparatus and production method using hydrogenated silicon chloride as a raw material.

  Monosilane is used as a raw material for high-purity silicon epitaxy, amorphous silicon, and the like, and is in great demand especially in various processes including manufacturing processes for semiconductors and solar cells, and is produced and supplied in large quantities as a liquefied gas. . In addition, for the production of monosilane, several production techniques have been proposed and put into practical use using hydrogenated silicon chloride as a raw material.

  For example, a solid catalyst such as an amine salt catalyst of a polymer sulfonic acid obtained by reaction of a strongly acidic cation exchange resin with an amine, an anion exchange resin catalyst having a tertiary amine group or a quaternary ammonium group in a reaction tower Is known, and a monosilane gas is produced by disproportionating dichlorosilane (see, for example, Patent Document 1). In addition, a mono-silane silane compound is continuously produced by using a tertiary aliphatic hydrocarbon-substituted amine and its hydrochloride as a catalyst for the disproportionation reaction and by performing a disproportionation reaction of silicon hydride chloride such as trichlorosilane. A method can be mentioned (for example, refer to Patent Document 2). Specifically, in the production apparatus as shown in FIG. 7, the raw material silicon hydride chloride is supplied to the reaction column 101 having the distillation function in which the disproportionation reaction catalyst is present, and the raw material is supplied from the upper part of the reaction column 101. Obtaining a silane compound with a lot of hydrogen atoms from silicon hydride chloride, extracting a mixed solution containing a silane compound with a lot of chlorine atoms and a catalyst from the bottom of the reaction tower 101, and then with the silane compound in the mixture solution The catalyst is separated and the separated catalyst is circulated to the reaction tower 101. Here, 102 is a reboiler, 103, 106 and 111 are condensers, 104 is a raw material supply conduit, 105 and 108 are control valves, 107 is a collection storage tank, 109 is a distillation tank, 110 is a pump, 112 is a storage tank, 113 is Indicates a replenishment bottle.

Patent Document 2 clearly states the following.
(A) Dichlorosilane, monochlorosilane, and monosilane are produced according to the disproportionation reaction formulas of the following formulas 1 to 3 (reversible reaction).
2SiHCl ₃ Ｓｉ SiCl ₄ + SiH ₂ Cl ₂ .. (Formula 1)
2SiH ₂ Cl ₂ Ｓｉ SiHCl ₃ + SiH ₃ Cl .. (Formula 2)
2SiH ₃ Cl Ｈ SiH ₂ Cl ₂ + SiH ₄・ ・ （Formula 3）
(B) Moreover, it is desirable that the ratio of the tertiary aliphatic hydrocarbon-substituted amine and its hydrochloride is 99 to 20 mol% for the former and 1 to 80 mol% for the latter. The reason is that if the latter ratio is less than 1 mol%, the catalytic action is small, and if it exceeds 80%, hydrochloric acid is released during the reaction to induce a reaction of the following formulas 4 to 7, This is because a silane compound having a large number of hydrogen atoms may not be obtained efficiently.
SiH ₄ + HCl → SiH ₃ Cl + H ₂ .. (Formula 4)
SiH ₃ Cl + HCl → SiH ₂ Cl ₂ + H ₂ .. (Formula 5)
SiH ₂ Cl ₂ + HCl → SiHCl ₃ + H ₂ .. (Formula 6)
SiHCl ₃ + HCl → SiCl ₄ + H ₂ .. (Formula 7)
(C) When the concentration of the hydrochloride of the tertiary aliphatic hydrocarbon-substituted amine in the catalyst is not a predetermined concentration, hydrogen chloride is replenished from the replenishment pipe 113 as necessary.

Japanese Patent No. 2648615 Japanese Patent Publication No. 64-003804

However, the following monosilane production methods sometimes cause various problems as described below.
(I) The conversion reaction to monosilane by the reaction using chlorosilane such as dichlorosilane as a raw material is an equilibrium reaction, and the equilibrium conversion rate is not necessarily as high as 10 to 18%. In order to obtain a desired production amount, A large device was needed.
(Ii) In addition, the reaction (a) involved in the production of the monosilane itself is required to control the concentration of the hydrochloride of the tertiary aliphatic hydrocarbon-substituted amine within a predetermined range. That is, hydrogen chloride plays a substantially catalytic role for forming the reaction (a). Therefore, as in (c) above, replenishment of hydrogen chloride is indispensable, and there is a problem that the handling becomes complicated.
(Iii) Furthermore, excessive supply of hydrogen chloride leads to generation of excess hydrogen by the reaction (b). The generation of hydrogen requires a separation process from monosilane at a later stage and causes a decrease in the yield of monosilane. In order to obtain a desired production amount, there is a problem that a large amount of trichlorosilane and dichlorosilane as raw materials are required. In addition, it is very difficult to remove hydrogen from a monosilane mixture containing hydrogen in particular because of the chemical properties of both, and a cryogenic apparatus using high pressure and liquid nitrogen is required to separate the hydrogen. There was a problem.

  An object of the present invention is to provide a monosilane that is capable of producing monosilane with a high yield of monosilane and a continuous and highly stable monosilane with a minimum amount of raw materials, without lowering the yield due to excessive reaction in the production process of monosilane. It is in providing a manufacturing apparatus and a manufacturing method.

  As a result of intensive studies to solve the above problems, the present inventors have found that the above object can be achieved by the monosilane production apparatus and production method described below, and have completed the present invention.

The apparatus for producing monosilane according to the present invention uses hydrogenated silicon chloride as a raw material, and uses a tertiary aliphatic hydrocarbon-substituted amine or / and a hydrochloride of a tertiary aliphatic hydrocarbon-substituted amine as a catalyst. A reaction tower to be produced, a separation device for extracting monosilane from a reaction product delivered from the upper stage of the reaction tower and separating it from a condensate comprising other components, and a tower bottom delivered from the lower stage of the reaction tower The liquid is heated, the hydrogenated silicon chloride contained in the column bottom liquid is evaporated to produce a concentrated liquid, and a part of the raw materials and / or a part of the condensed liquid is added to the concentrated liquid. And a catalyst regeneration tank in which the catalyst contained in the concentrate is reactivated and a regeneration solution containing the catalyst is prepared.
The regeneration solution supplied from the catalyst regeneration tank is supplied to the reaction tower to form a circulation system related to the catalyst.

  In the conventional monosilane production process, it is indispensable to supply hydrogen chloride in order to maintain the catalytic activity, and the supply of excess hydrogen chloride has caused various problems associated with the generation of hydrogen. As a result of verifying the function of such a catalyst, the present inventor found that not only hydrogen chloride but also the catalyst concentration is high (concentration) and under conditions exceeding a predetermined temperature, for example, monochlorosilane, dichlorosilane, etc. It has also been found that sufficient reactivation (regeneration) can be achieved by the components contained in the hydrogenated silicon chloride. In other words, a catalyst regeneration tank that can be heated by adding a part of the raw material and / or a part of the condensate to the concentrated liquid in which the used catalyst is concentrated is provided, and the reactivated catalyst is again brought into the reaction tower at a high temperature. By forming a circulation system related to the catalyst, it is not necessary to supply hydrogen chloride from the outside, and it is not accompanied by generation of hydrogen that has caused various problems, and with minimal raw materials. The yield of monosilane is high, and it has become possible to produce monosilane that is continuous and highly stable. Monochlorosilane, dichlorosilane, etc. are generated or exist not only in the raw material but also in the intermediate stage of the production process. By effectively using this, the catalytic reaction can be promoted more efficiently. It was possible to produce monosilane with high yield. Furthermore, the reactivation reaction in the catalyst regeneration tank is a reaction for producing monosilane from monochlorosilane, dichlorosilane or the like in the raw material or condensate, and if the reaction in the reaction tower is a secondary reaction, The primary reaction is performed, and it becomes possible to produce monosilane with higher yield. As will be described later, the separation device may be configured by a rectifying column or a plurality of stages of condensers whose set temperatures are successively reduced.

  The present invention is the above-described monosilane production apparatus, wherein the catalyst regeneration tank includes a first regeneration tank to which a part of the raw material is supplied and a second regeneration tank to which a part of the condensate is supplied. After the concentrated liquid is supplied to one of the first regeneration tank and the second regeneration tank, the liquid supplied from one of the regeneration tanks is further supplied to another regeneration tank to produce a regeneration liquid. It is characterized by that.

  As described above, it has been found that reactivation of the catalyst in the catalyst regeneration tank is possible with either the raw material or the condensate. However, along with the difference in composition between the two, the function or technical effect in the catalyst regeneration tank provided immediately before the reaction tower for both differs. Therefore, these functions can be utilized more effectively by constituting independent catalyst regeneration tanks and arranging them in series. That is, in a configuration comprising two regeneration tanks, when the raw material is supplied to the upstream regeneration tank, the catalyst regenerated upstream contacts the condensate downstream, and unreacted components in the condensate are removed. It is converted to monosilane or the like by reaction again. On the other hand, when the condensate is supplied to the regeneration tank on the upstream side, the catalyst regenerated on the upstream side promotes a new reaction of the raw material on the downstream side. That is, if the reaction in the reaction tower is a secondary reaction, the primary reaction is performed in the downstream regeneration tank. In addition, each configuration has the function and effect of improving the yield of monosilane, but either can be selected depending on the composition of the raw material or the condensate, and a higher yield can be achieved. .

  The present invention is the above-described monosilane production apparatus, wherein the separation device is composed of a plurality of separation tanks whose set temperatures are successively reduced, and the reaction product is the uppermost separation tank under the highest temperature condition. And a part of the condensate discharged from each separation tank is supplied to at least one of the catalyst regeneration tank, the evaporation tank, and the reaction tower. It is characterized by being.

  In the disproportionation reaction of hydrogenated silicon chloride, it is known that the reaction rate increases as the number of chlorines decreases, such as monochlorosilane> dichlorosilane> trichlorosilane ("Low-Cost Solar Array Project Report" 175 Page, published in June 1979 (Union Carbide Corporation): NASA-CR-162172 etc.). In the verification relating to the catalyst reactivation function of the present inventor, it was found that the same tendency can be estimated. In addition, the boiling point of each substance increases in the order of monochlorosilane (bp about −30 ° C.), dichlorosilane (bp about 8 ° C.), and trichlorosilane (bp about 32 ° C.). Based on these findings, the present invention uses a separation apparatus comprising a plurality of separation tanks whose set temperatures are successively reduced in the extraction of monosilane from the reaction product and the generation of condensate for the remaining other components. It is possible to re-activate the catalyst more efficiently by taking out the condensate containing a large amount of monochlorosilane, dichlorosilane, etc., which has a high reactivation function, and supplying it to the catalyst regeneration tank. became. In the evaporation tank, the column bottom liquid containing hydrogenated silicon chloride having a low catalyst reactivation function is heated to produce a concentrated liquid containing the catalyst under high temperature conditions. However, if the condensate containing a large amount of monochlorosilane, dichlorosilane or the like having a high reactivity of the highly reactive catalyst exists in the evaporation tank, the inventor will reactivate the catalyst in the same manner as in the catalyst regeneration tank. The knowledge that it is possible to carry out the conversion process was obtained. On the other hand, in a separation apparatus composed of a plurality of stages of separation tanks whose set temperatures are successively lowered, such condensate can be taken out from the plurality of stages of separation tanks. The present invention performs the primary reactivation treatment of the catalyst in the evaporation tank by supplying the condensate supplied from the separation tank to the evaporation tank instead of the catalyst regeneration tank, and further in the catalyst regeneration tank. The secondary reactivation treatment can be performed, and the reactivated catalyst function can be utilized in the reaction tower. In addition, since the condensate from the multistage separation tank contains unreacted components such as monochlorosilane and dichlorosilane, the yield of monosilane can be increased by supplying it again to the reaction tower. . Furthermore, such condensate can be supplied to the catalyst regeneration tank, evaporation tank and reaction tower in parallel, and the temperature of each separation tank (condensate composition fluctuates) and separation can be performed. It is also possible to set a supply destination for each different condensate according to the composition of the condensate from the tank. The present invention has an unprecedented feature in that the method of using the condensate supplied from the plurality of separation tanks can be applied in various ways according to required specifications.

  The present invention provides the above-described monosilane production apparatus, wherein a lower-stage cooler for cooling the hydrogenated silicon chloride evaporated and delivered from the evaporation tank is provided with a plurality of stages of coolers whose set temperatures are successively lowered. The exhaust liquid condensed in the first cooler at the most upstream stage is taken out, and the vapor phase components separated in the first cooler are sequentially transferred to the coolers in the next stage and at least in each cooler. The liquid condensed in one is supplied to the catalyst regeneration tank as a part of the condensed liquid.

  As for the bottom liquid from the conventional reaction tower, the concentrated liquid containing the catalyst concentrated in the evaporation tank is supplied to the reaction tower, and the vapor phase component separated in the evaporation tank is further cooled in the lower cooler to be tetrachlorosilane. It was only recovered as a recovering liquid mainly composed of However, the gas phase component includes trichlorosilane and dichlorosilane in addition to the main component tetrachlorosilane. Therefore, if dichlorosilane or the like in the gas phase component can be extracted, it can be used for the reactivation process. The present invention is composed of two or more coolers that are sequentially subjected to low-temperature processing as the lower cooler, and the gas phase component separated in the first cooler at the uppermost stream is further cooled by a cooler at a lower temperature downstream. By supplying the condensed liquid as a part of the condensate to the catalyst regeneration tank and again supplying it to the reaction tower, the yield of monosilane can be increased.

In addition, the present invention provides a method for producing monosilane, characterized in that monosilane is produced by the following steps using any of the monosilane production apparatuses described above.
(1) Monosilane in the presence of a catalyst comprising a tertiary aliphatic hydrocarbon-substituted amine or / and a tertiary aliphatic hydrocarbon-substituted amine hydrochloride, wherein the raw material hydrogenated silicon chloride is supplied to the reaction tower A reaction product containing
(2) The reaction product delivered from the upper stage of the reaction tower is supplied to a separation device, separated into monosilane and a condensate, and the monosilane is taken out.
(3) The tower bottom liquid supplied from the lower stage of the reaction tower is supplied to the evaporation tank and heated, and the silicon hydride chloride contained in the tower bottom liquid is evaporated to produce a concentrated liquid.
(4) The concentrated liquid is supplied to a catalyst regeneration tank, heated by adding a part of the raw material and / or a part of the condensate separated by the separator, and the catalyst contained in the concentrated liquid Reactivated again to make a regenerating solution,
(5) The regeneration solution is supplied to the reaction tower to form a circulation system related to the catalyst.

  With such a configuration, it is possible to form a monosilane production method capable of producing monosilane having high energy efficiency, high yield, and continuous and high stability without using complicated operations.

  The present invention provides the above-described monosilane production method, wherein at the time of start-up, the catalyst and a part of the raw material are supplied to the catalyst regeneration tank, the catalyst is initially activated, and the treatment is performed. The broken catalyst solution and the raw material are supplied to the reaction tower.

  In various processes such as semiconductor manufacturing processes, it is sometimes required to start monosilane supply promptly as well as to periodically stop monosilane. As one of the rate-determining factors for such activation, initial activation of the catalyst is required. Can be mentioned. In the present invention, the catalyst and a part of the raw material are supplied to the catalyst regeneration tank to perform the initial activation treatment of the catalyst, which is quicker than the conventional method requiring the addition of hydrogen chloride. There was no supply or generation of hydrogen, and it became possible to meet these demands. In addition, it is possible to further speed up the process by supplying monosilane produced by the initial activation treatment of the catalyst using a part of the raw material.

Schematic which shows the 1st structural example of the manufacturing apparatus of the monosilane which concerns on this invention. Schematic which shows the 2nd structural example of the manufacturing apparatus of the monosilane which concerns on this invention. Schematic which shows the 3rd structural example of the manufacturing apparatus of monosilane which concerns on this invention. Schematic which shows the 4th structural example of the manufacturing apparatus of the monosilane which concerns on this invention. Schematic illustrating the time until the disproportionation reaction reaches equilibrium when the reaction temperature is changed Schematic illustrating the time until the disproportionation reaction reaches equilibrium when the reaction temperature is changed Schematic illustrating a monosilane production method apparatus according to the prior art

  The apparatus for producing monosilane according to the present invention (hereinafter referred to as “the present apparatus”) uses at least a tertiary aliphatic hydrocarbon-substituted amine and / or a tertiary aliphatic hydrocarbon-substituted amine using hydrogenated silicon chloride as a raw material. A reaction tower in which monosilane is produced using hydrochloride as a catalyst, a separation apparatus in which monosilane is extracted from a reaction product provided from the upper stage of the reaction tower and separated from a condensate composed of other components, and a reaction A column bottom liquid delivered from the lower stage of the column is heated, a hydrogenated silicon chloride contained in the column bottom liquid is evaporated to produce a concentrated liquid, a part of the raw material in the concentrated liquid and / or A catalyst regeneration tank in which a part of the condensate is added and heated, the catalyst contained in the concentrate is reactivated, and a regeneration liquid containing the catalyst is prepared, and is supplied from the catalyst regeneration tank. Regenerated liquid is supplied to the reaction tower. Characterized in that the circulatory system according to the catalyst is formed. There is no need to supply hydrogen chloride from the outside, and there is no generation of hydrogen that has caused various problems, and the yield of monosilane is high with minimal raw materials, and it is continuous and highly stable. An apparatus for producing monosilane can be provided. Hereinafter, embodiments of the present invention will be described with reference to the drawings.

<Basic configuration example of this device>
An outline of a basic configuration example of the present apparatus is shown in FIG. 1 (first configuration example). This apparatus uses a tertiary aliphatic hydrocarbon-substituted amine or / and a hydrochloride of a tertiary aliphatic hydrocarbon-substituted amine as a catalyst (hereinafter sometimes referred to as “amine-based catalyst”), and is a raw material hydrochlorination. Reaction tower 1 in which monosilane is produced from silicon, separation apparatus 2 from which the monosilane is extracted and separated from the condensate, and tower bottom liquid delivered from reaction tower 1 are heated to produce a concentrate. A tank 3 and a catalyst regeneration tank 5 in which a part of the raw material and / or part of the condensate is added to the concentrated liquid and heated to produce a regenerated liquid containing the regenerated catalyst. Further, a concentrated liquid containing a catalyst obtained by concentrating the bottom liquid containing the catalyst delivered from the reaction tower 1 in the evaporation tank 3 is fed to the catalyst regeneration tank 5 by the feed pump 4. The supplied regenerated liquid is supplied to the reaction tower 1 to form a circulation system related to the catalyst. There is no need to supply hydrogen chloride for catalyst regeneration from the outside, and there is no generation of hydrogen which has caused various problems. Highly stable monosilane can be produced. Here, “silicon hydride chloride” used as a raw material in the present production process refers to any of monochlorosilane, dichlorosilane, trichlorosilane, and tetrachlorosilane, or a combination thereof.

In this apparatus, monosilane is produced by the following steps (hereinafter referred to as “the present method”).
(1) Hydrogenated silicon chloride as a raw material is supplied to the reaction tower 1, and in the presence of a catalyst comprising a tertiary aliphatic hydrocarbon-substituted amine or / and a tertiary aliphatic hydrocarbon-substituted amine hydrochloride, A reaction product containing monosilane is produced,
(2) The reaction product delivered from the upper stage 1c of the reaction tower 1 is supplied to the separation device 2, separated into monosilane and a condensate, and the monosilane is taken out.
(3) The tower bottom liquid delivered from the lower stage 1b of the reaction tower 1 is supplied to the evaporation tank 3 and heated, and the silicon hydride chloride contained in the tower bottom liquid is evaporated to produce a concentrated liquid.
(4) The concentrated liquid is supplied to the catalyst regeneration tank 5 and heated by adding a part of the raw material or / and a part of the condensate separated by the separation device 2 to recycle the catalyst contained in the concentrated liquid. Activated to produce a regenerating solution,
(5) The regenerated liquid is supplied to the reaction tower 1 to form a circulation system related to the catalyst.
Hereinafter, the function and each process of this apparatus will be described in detail.

(1) Production of reaction product in the reaction tower 1 Liquid hydrogenated silicon chloride as a raw material is supplied to the reaction tower 1. By heating the raw material in advance, the reaction rate in the reaction tower 1 can be increased. The supplied raw material is reacted in the presence of an amine catalyst supplied in advance in the tower bottom 1b heated to a reaction temperature of about 100 to 150 ° C. by a heating means (reboiler 1a) (hereinafter referred to as “monosilane production reaction”). May be converted to a reaction product comprising monosilane and reaction or containing unreacted silicon hydride chloride. In the reaction tower 1, such a reaction and separation by distillation occur simultaneously, and among the reaction products, low-boiling components such as monosilane and monochlorosilane rise in the reaction tower 1 and are fed from the upper stage 1c to the separation device 2. The At this time, it is preferable to cool such an upward flow in the middle and upper stages of the reaction tower 1 to liquefy the component having a relatively high boiling point and return it to the tower bottom 1b to be used for the reaction again. The reaction tower 1 is supplied with an amine catalyst that has been reactivated and heated in the catalyst regeneration tank 5. Due to the always active catalyst, the yield of monosilane in the reaction product can be kept high. As the reaction tower 1, for example, a rectification tower made of stainless steel can be used. In addition, for example, a sieve tray can be used for the multi-stage rectification stage.

  The reaction in the reaction tower 1 is formed based on a disproportionation reaction formula such as the above formulas 1 to 3 of (a), and tetrachlorosilane, trichlorosilane, dichlorosilane, monochlorosilane, and monosilane are generated (monosilane or the like). Production reaction). Here, since the reaction system constitutes a reversible reaction, when only the produced monosilane is taken out, the production reaction of monosilane from monochlorosilane proceeds reversibly based on the above formula 3 as the amount of monosilane is reduced. . Therefore, the yield of monosilane can be increased by returning the condensed liquid obtained by extracting monosilane from the reaction product or the hydrogenated silicon chloride evaporated in the evaporation tank 3 to the reaction system again.

  The catalyst is preferably an amine-based catalyst, specifically, a tertiary aliphatic hydrocarbon-substituted amine such as trioctylamine or tributylamine or a hydrochloride of a tertiary aliphatic hydrocarbon-substituted amine, and a mixture thereof. More preferred. In particular, the presence of a hydrochloric acid group can maintain a high catalytic activity in this reaction system. On the other hand, such amine-based catalysts are gradually reduced in catalytic activity by repeating the disproportionation reaction of hydrogenated silicon chloride (formation reaction of monosilane, etc.), so it is necessary to reactivate and regenerate. As described above, knowledge of such catalytic activity could be obtained by contacting monochlorosilane or dichlorosilane in the raw material or reaction product with the catalyst under heating conditions. In this apparatus, it is possible to maintain the presence of hydrochloric acid groups indispensable for catalyst activity by such reactivation treatment without adding conventional hydrogen chloride. Specifically, a column bottom liquid containing an amine-based catalyst is supplied from the lower stage of the reaction tower 1 and concentrated with a high-boiling high-concentration amine-based catalyst prepared by evaporating silicon hydride chloride in the evaporation tank 3. The catalyst was reactivated by adding the concentrate and part of the raw material or / and part of the condensate in the catalyst regeneration tank 5 that was prepared and heated to about 100 to 150 ° C. The regenerated liquid containing is again supplied to the reaction tower 1. By forming such a circulation system for the catalyst, the reaction tower 1 always has an amine catalyst having a high catalytic activity. Therefore, the yield of monosilane in the reaction product can be kept high.

(2) Extraction of Monosilane and Separation of Condensate in Separation Device 2 The reaction product (about 50 to 100 ° C.) delivered from the reactor 1 is extracted with monosilane in the separation device 2 and is condensed with other components. To be separated. The reaction product supplied to the separation device 2 includes a low-boiling monosilane (bp about −112 ° C.), a high-boiling monochlorosilane (bp about −30 ° C.) and dichlorosilane (bp about −bp). Hydrogenated silicon chloride such as 8 ° C) is mixed. Thus, since the difference in boiling point between monosilane to be separated and other components is large, it can be extracted as monosilane with high purity at the product level. As the separation device 2, for example, a configuration in which monosilane is taken out by a single device, such as a rectification column or a single low-temperature condenser, or a configuration including a plurality of condensers in which the set temperature is sequentially reduced is used. be able to. When a rectification column is used, the boiling points of monosilane and other components are greatly different, so multiple rectification stages are not required, and a sufficient separation function can be ensured with a relatively simple structure. it can. Monosilane having a temperature of about −20 to −30 ° C. and a pressure of about 0.2 to 1 MPa is supplied from the top of the rectifying tower, and a condensate having a temperature of about 50 to 100 ° C. and a pressure of about 0.2 to 1 MPa is supplied from the bottom of the tower. Is done. Since high catalytic activity can be maintained, there are many low-boiling substances such as monosilane in the condensate, and separation can be performed with a higher yield under low-pressure conditions than before. Similarly, a refrigerant such as liquid nitrogen (reachable temperature of about −196 ° C.) or ethanol / dry ice (reachable temperature of about −72 ° C.) is also used when a single-stage low-temperature condensing tank (heat exchanger) is used. Can be used to deliver monosilane and condensate with similar properties. Furthermore, the separation device 2 can be configured not only with a single condensing tank but also with a multistage condensing tank. By sequentially lowering the cooling temperature, each condensing tank can be efficiently cooled. Details will be described later. In the first configuration example, such a structure is not limited, and the monosilane is shown as an integrated separation device 2 that separates monosilane from condensate composed of other components.

  The condensate delivered from the separator 2 is mainly composed of low-boiling silicon hydride chloride such as monochlorosilane or dichlorosilane, and can be returned to the reaction tower 1 again to contribute to the production of monosilane (not shown). ). In this apparatus, the low-boiling silicon hydride chloride is further provided with a regeneration function of an amine catalyst, and is supplied to the catalyst regeneration tank 5 to contribute to the catalyst reactivation process. . Further, as will be described later, the evaporation tank 3 constituting this apparatus has conditions similar to the catalyst regeneration tank 5 such as the heating temperature and the presence of the concentrated catalyst, and therefore the presence of monochlorosilane, dichlorosilane or the like is present. If there is, it is possible to carry out the reactivation process, so that a part of the condensate can be supplied to the evaporation tank 3 to contribute to the catalyst reactivation process here. As described above, the condensate supplied from the separation device 2 can not only re-react the conventional unreacted components but also effectively use the composition to ensure a high yield of monosilane.

(3) Preparation of concentrated liquid in evaporation tank 3 and separation of silicon hydride chloride The bottom liquid containing a high-boiling amine catalyst delivered from the lower stage 1b of the reaction tower 1 is adjusted to a set flow rate by a control valve 7. , And supplied to the evaporation tank 3. In the evaporation tank 3, the hydrogenated silicon chloride is evaporated to produce a concentrated liquid containing a high concentration amine-based catalyst. The tower bottom liquid is mainly composed of high boiling silicon hydride chloride such as tetrachlorosilane together with the catalyst. The evaporation tank 3 is operated at a temperature higher than the boiling point (about 32 ° C. or higher) of the high boiling silicon hydride chloride such as tetrachlorosilane generated by the disproportionation reaction and lower than the boiling point of the catalyst (about 160 to 220 ° C.). Is done. In order to prevent thermal decomposition of the catalyst, the temperature is preferably low, and specifically, it is preferably heated by a heating means (reboiler 3a) and operated at about 80 to 120 ° C. Tetrachlorosilane and the like evaporated in the evaporation tank 3 are condensed in the lower cooler 6 and then stored and recovered in the storage tank 6a. The gas phase component separated by the lower cooler 6 is discharged out of the system, or cooled and separated again as described later and reused. The concentrated liquid containing the catalyst remaining in the evaporation tank 3 is extracted by the feed pump 4, fed to the catalyst regeneration tank 5, subjected to reactivation, and then used again for the disproportionation reaction.

(4) Catalyst Reactivation Treatment in the Catalyst Regeneration Tank 5 The catalyst regeneration tank 5 includes a heating means (reboiler 5a) for heating and a stirring means (not shown). In the catalyst regeneration tank 5, a part of the raw material or / and a part of the condensate separated by the separation device 2 are added to the supplied concentrate, and the mixture is stirred under heating conditions. The catalyst contained in is reactivated. In other words, under conditions where the concentration of the catalyst is high and exceeds a predetermined temperature, the catalyst and chloride ions required for the catalytic activity estimated by the silicon hydride chloride such as monochlorosilane and dichlorosilane can be used without using hydrogen chloride. It was found that the formation of a conjugate with (radical) can be sufficiently ensured. Specifically, in the catalyst regeneration tank 5 heated to a processing temperature of about 100 to 150 ° C., the concentrated amine-based catalyst and monochlorosilane, dichlorosilane, or the like are stirred and mixed to be activated at the initial stage. A catalyst structure similar to the catalyst can be formed. Monochlorosilane, dichlorosilane, or the like as a substrate for such reactivation is a monochlorosilane extracted from a condensate or a raw material having such a composition, or from an effluent separated in an evaporation tank 3 to be described later, in this manufacturing process. Or dichlorosilane can be used. The regenerated liquid containing the reactivated catalyst is supplied to the upper part of the reaction tower 1 in a heated state.

  At this time, a catalyst regeneration tank 5 that can be heated by adding a part of the raw material or / and a part of the condensate to the concentrated liquid in which the used catalyst is concentrated is provided, and the reactivated catalyst is reacted again in a high temperature state. A catalyst-related circulation system is formed that returns to the column. There is no need to supply hydrogen chloride from the outside, and there is no generation of hydrogen that has caused various problems, and the yield of monosilane is high with minimal raw materials, and it is continuous and highly stable. Monosilane can be produced. Monochlorosilane, dichlorosilane, etc. are generated or exist not only in the raw material but also in the intermediate stage of the production process. By effectively using this, the catalytic reaction can be promoted more efficiently. And high yield monosilane can be produced. Furthermore, in the catalyst regeneration tank 5, a part of monochlorosilane, dichlorosilane, etc. is a silicon hydride chloride having a new composition containing monosilane by a production reaction of monosilane such as the above formulas 1-3 of (a). Form. That is, when viewed from the production process of monosilane, the catalyst regeneration tank 5 undergoes the primary reaction, and the monosilane having higher yield can be produced through the secondary reaction in the reaction tower 1. As described above, it can be said that the catalyst regeneration tank 5 in the present apparatus has a function of performing a reactivation process of the catalyst and simultaneously performing a process as a primary reaction for producing monosilane.

  Further, the catalyst regeneration tank 5 can exhibit a useful function when the present apparatus is activated. That is, as the initial operation of this apparatus, the catalyst and a part of the raw material are supplied to the catalyst regeneration tank 5 so that the initial activation process of the catalyst can be performed in the same manner as the reactivation process. By supplying the catalyst liquid and the raw material subjected to such treatment to the reaction tower 1, it is possible to quickly perform a monosilane production reaction in the reaction tower 1, and to quickly start up the supply of monosilane. . In particular, the primary reaction of the raw material in the catalyst regeneration tank 5 also contributes to this. For the initial activation of the catalyst, which is one of the rate-determining factors for the start-up in the monosilane supply process, the catalyst regeneration tank 5 is used to perform the initial activation treatment of the catalyst, thereby adding the conventional hydrogen chloride. Compared to the required method, it is quicker and does not supply hydrogen chloride or generate hydrogen, making it possible to meet these demands.

(5) Supply of the regenerated liquid to the reaction tower 1 (formation of a circulation system related to the catalyst)
The tower bottom liquid delivered from the reaction tower 1 is concentrated in the evaporation tank 3, the catalyst contained in the catalyst regeneration tank 5 is reactivated, and is supplied again to the reaction tower 1 as a regeneration liquid. The catalyst used in the evaporation tank 3 is concentrated, and in the catalyst regeneration tank, monochlorosilane, dichlorosilane or the like is added to the concentrated liquid to heat and reactivate the catalyst, and the reactivated catalyst is again in a high temperature state. Thus, a circulation system related to the catalyst is formed, which is returned to the reaction tower. By forming such a circulation system related to the catalyst, there is always an amine-based catalyst having a high catalytic activity in the reaction tower 1, and there is no need to supply hydrogen chloride from the outside, and hydrogen generation is involved. In addition, the yield of monosilane is high with a minimum amount of raw materials, and it is possible to produce monosilane continuously and highly stable.

<Other configuration examples of the apparatus>
As described above, this apparatus can have many unprecedented functions as a whole system by including the constituent elements having various functions such as the catalyst regeneration tank 5, and further include additional functions. Configuration examples can be developed.

[Second configuration example of this apparatus]
As another example of the configuration of the present apparatus, an outline of an apparatus in which the catalyst regeneration tank 5 includes a plurality of regeneration tanks is illustrated in FIGS. 2A and 2B (second configuration example). In the first configuration example, the catalyst regeneration tank 5 includes a first regeneration tank (51 or 52) to which a part of the raw material is supplied and a second regeneration tank (52 or 51) to which a part of the condensate is supplied. It consists of. After the concentrated liquid is supplied to either the first regeneration tank (51 or 52) or the second regeneration tank (52 or 51), the liquid supplied from one of the regeneration tanks is further supplied to another regeneration tank. In addition, by producing the regenerating liquid, it is possible to have an excellent function different from the case where a single regenerating tank is used. Both the raw material and the condensate are useful for reactivation of the catalyst, but the functions or technical effects in the reactivation treatment are different because the compositions of monochlorosilane and dichlorosilane contained therein are different. Therefore, these functions can be utilized more effectively by constituting independent catalyst regeneration tanks and arranging them in series. In addition, each configuration has the function and effect of improving the yield of monosilane, but either can be selected depending on the composition of the raw material or the condensate, and a higher yield can be achieved. . Here, two configurations illustrated in FIGS. 2A and 2B will be described in detail.

  Specifically, the first regeneration tank 51 to which a part of the raw material is supplied is arranged on the upstream side, and the second regeneration tank 52 to which a part of the condensate is supplied is arranged on the downstream side. As shown in FIG. Part of the raw material is supplied to the first regeneration tank 51 together with the concentrated liquid via the channel La, and both are stirred and mixed in the first regeneration tank 51, and the catalyst in the concentrated liquid is obtained by silicon hydride chloride in the raw material. Is reactivated. Next, the reactivated catalyst is transferred from the first regeneration tank 51 to the second regeneration tank 52 on the downstream side. In the second regeneration tank 52, the second regeneration tank 52 is passed from the separation device 2 through the flow path Lc. A part of the raw material and silicon hydride chloride in the condensate is converted to monosilane or the like by a production reaction such as monosilane. At this time, in the first regeneration tank 51, a high catalyst reactivation function can be obtained due to the presence of unreacted monochlorosilane, dichlorosilane, or the like in the raw material. In addition, the hydrogenated silicon chloride in the raw material is in the presence of a catalyst with reduced reactivity, and the rate of conversion to monosilane or the like is not high, but in the second regeneration tank 52, the reactivated catalyst In the presence, part of it is converted to monosilane or the like. The reactivation function of the catalyst in the first regeneration tank 51 on the upstream side can be enhanced, and the high reactivity of the production reaction such as monosilane in the reaction tower 1 and the second regeneration tank 52 on the downstream side can be ensured. At this time, by setting the two regeneration tanks 51 and 52 to different set temperatures, the respective functions are enhanced, and the reactivation process and the primary reaction process in the second regeneration tank 52 are performed more effectively. be able to. For example, the reactivation temperature in the first regeneration tank 51 is heated to about 100 to 150 ° C., and the second regeneration tank 52 is heated to about 80 to 120 ° C. that is slightly lower than the monosilane production reaction temperature. The regenerating liquid can be supplied to the reaction tower 1 so as not to overheat while ensuring the reactivation process and the primary reaction process.

  On the other hand, FIG. 2 shows a configuration in which a first regeneration tank 51 to which a part of the condensate is supplied is disposed on the upstream side, and a second regeneration tank 52 to which a part of the raw material is supplied is disposed on the downstream side. Shown in (B). A part of the condensate from the separation device 2 is supplied to the first regeneration tank 51 together with the concentrated liquid via the flow path Lc, and both are stirred and mixed in the first regeneration tank 51, and silicon hydride chloride in the raw material Thereby reactivating the catalyst in the concentrate. Next, the reactivated catalyst is transferred from the first regeneration tank 51 to the second regeneration tank 52 on the downstream side, and is supplied to the second regeneration tank 52 via the flow path La in the second regeneration tank 52. A part of the raw material comes into contact, and a part of silicon hydride chloride in the raw material is mainly converted into monosilane or the like by a production reaction such as monosilane (primary reaction). At this time, in the first regeneration tank 51, the catalyst reactivation function can be obtained by the presence of monochlorosilane, dichlorosilane, or the like in the condensate, but the first regeneration having the configuration shown in FIG. It may not be as high as the catalyst reactivation function in the tank 51. In the second regeneration tank 52, a part of the hydrogenated silicon chloride in the raw material is converted to monosilane or the like in the presence of the reactivated catalyst. Due to the reactivation function of the catalyst in the first regeneration tank 51 on the upstream side, the reactivity of monosilane and the like in the reaction tower 1 and the second regeneration tank 52 on the downstream side, particularly with respect to silicon hydride chloride in the raw material is high. Can be secured.

[Third configuration example of the apparatus]
As another configuration example of the present apparatus, in the first and second configuration examples, the separation device 2 has a plurality of separation tanks (in this case, the first separation tank 21 of the second stage, FIG. 3 shows an outline of an apparatus composed of two separation tanks 22 and three or more separation tanks 23, 24,. In the separation device 2 including the first separation tank 21 and the second separation tank 22, the reaction product is supplied to the first separation tank 21 in the uppermost stream stage at the highest temperature condition and sequentially transferred to the second separation tank 22. At the same time, a part of the condensate supplied from at least one of the first and second separation tanks 21 and 22 is supplied to at least one of the catalyst regeneration tank 5, the evaporation tank 3, and the reaction tower 1. As described above, in the catalyst reactivation function, as in the disproportionation reaction of hydrogenated silicon chloride, it is estimated that the smaller the number of chlorine, the higher the reaction rate (monochlorosilane>dichlorosilane> trichlorosilane). I learned that I can do it. Based on this knowledge, using the separation device 2 composed of the first and second separation tanks 21 and 22 in which the set temperature is gradually reduced, monochlorosilane, dichlorosilane, etc. having a high reactivity catalyst reactivation function, etc. By removing the condensate containing a large amount and supplying it to at least one of the catalyst regeneration tank 5, the evaporation tank 3 and the reaction tower 1, the catalyst can be reactivated more efficiently.

  For example, the first separation tank 21 is cooled using cooling water at about 10 ° C. as a refrigerant, and the second separation tank 22 is cooled using ethanol / dry ice (attainable temperature of about −72 ° C.) as a refrigerant. Assuming that, the function will be explained. It is assumed that a condensate mainly composed of trichlorosilane is formed from the first separation tank 21, and a condensate mainly composed of monochlorosilane and dichlorosilane is formed from the second separation tank 22. However, it goes without saying that the number of separation tanks, the set temperature, the composition of the condensate, and the like are not limited thereto.

  At this time, the catalyst can be reactivated more efficiently by the configuration in which the condensate from the second separation tank 22 is supplied to the catalyst regeneration tank 5 and / or the evaporation tank 3. That is, the condensate from the second separation tank 22 is supplied to the catalyst regeneration tank 5 via the flow path Lc as in the first configuration example, so that the catalyst and the condensate are heated in the catalyst regeneration tank 5 at a high temperature. The catalyst can be reactivated by stirring and mixing under conditions. Further, by supplying the condensate from the second separation tank 22 to the evaporation tank 3 via the flow path Lv, the concentrated liquid containing the catalyst and the condensate are mixed under high temperature conditions, and the catalyst is reactivated. It can be performed. In order to verify the function of the evaporating tank 3 in the present apparatus, the evaporating tank 3 contains a concentrated liquid containing a catalyst under a high temperature condition. At this time, if monochlorosilane, dichlorosilane, or the like is supplied to the evaporation tank 3, the catalyst can be reactivated as in the catalyst regeneration tank 5. Therefore, by supplying the condensate from the second separation tank 22 to the evaporation tank 3, the catalyst is substantially subjected to primary reactivation in the evaporation tank 3, and further subjected to secondary reactivation in the catalyst regeneration tank 5. The reaction function can be utilized, and the reactivated catalyst function can be utilized in the reaction tower 1.

  Moreover, the yield of a higher monosilane can be obtained by supplying the condensate from the 1st separation tank 21 or / and the 2nd separation tank 22 to the reaction tower 1 via the flow path Lr. Since the condensate excluding monosilane extracted in the separation apparatus 2 contains unreacted components such as monochlorosilane, dichlorosilane, and trichlorosilane, the monosilane is recovered by supplying it to the reaction tower 1 again. You can raise the rate.

  Furthermore, by supplying the condensate from the first separation tank 21 to the evaporation tank 3, it is possible to efficiently produce monosilane. That is, when the condensate from the first separation tank 21 is refluxed to the catalyst circulation system or the reaction tower 1, the yield of monosilane is increased, but the condensate mainly composed of trichlorosilane having a slow reaction rate is used. Presence may reduce the reaction efficiency in the production reaction of monosilane and the like. Accordingly, such a condensate is supplied to the evaporation tank 3, separated by the lower cooler 6, discharged or condensed as a gas phase component, stored in the storage tank 6a, recovered, and fed out of the system. It is possible to reduce the reaction load in the isogenic reaction and improve the reaction efficiency.

[Fourth configuration example of this apparatus]
As another configuration example of the present apparatus, as the lower cooling unit 6 for separating the silicon hydride chloride evaporated and supplied from the evaporation tank 3, a plurality of coolers (first coolers 61, An outline of the apparatus having the second cooler 62) is shown in FIG. 4 (fourth configuration example). In the first configuration example, the silicon hydride vaporized and delivered from the evaporation tank 3 is supplied to the first cooler 61 at the uppermost stream, and the discharged liquid condensed in the first cooler 61 is stored in the storage tank 61a. The vapor phase component that is taken out after being separated and separated in the first cooler 61 is transferred to a second cooler 62 that is cooled at a lower temperature after the next stage, and condensed in the second cooler 62. Is supplied to the catalyst regeneration tank 5 as part of the condensate. The discharged liquid condensed in the second cooler 62 is taken out after being stored in the storage tank 62a. That is, since the vapor phase component separated in the evaporation tank 3 includes dichlorosilane and the like in addition to trichlorosilane, it can be used for the reactivation process. The yield of monosilane can be increased.

<Verification of this device and this method>
The functions and technical significance of the present apparatus and the present method including the above-described configuration examples were compared and verified with conventional methods. The details will be described below.

[Verification experiment 1]
(1) Experimental conditions of verification experiment 1 Trichlorosilane as a raw material, n-trioctylamine as an amine catalyst, a 500 cc autoclave equipped with a stirrer and a heater as a reactor (corresponding to a reaction tower), a raw material and an amine catalyst Was introduced into the reactor, and in a sealed state, a disproportionation reaction was performed under a reaction pressure of 2 to 3 bar and the following temperature conditions. The amount of catalyst used was unified at a molar ratio of 10% with respect to the raw material trichlorosilane. Since the amount of trichlorosilane in the gas phase of the reactor corresponds to the conversion rate of trichlorosilane, when the disproportionation reaction reaches an equilibrium state, the amount of trichlorosilane becomes a predetermined value, so that the reaction temperature is 50-100. The time until the disproportionation reaction reached an equilibrium state when the temperature was changed to ° C. was verified. The content of chlorosilanes in the gas phase of the reactor was quantitatively measured by FT-IR.

(2) Experimental conditions of Comparative Experiment 1 In Comparative Experiment 1, the same raw materials, amine catalyst and reactor as those in Verification Experiment 1 were used, and an operation of adding hydrogen chloride (HCl) to the catalyst was added. The disproportionation reaction was performed under the conditions, and the time until the disproportionation reaction reached an equilibrium state when the reaction temperature was changed to 50 to 100 ° C. was verified. The reaction for adding HCl was performed by introducing an amine catalyst into the reactor, then introducing HCl into the reactor, discharging excess HCl, and then introducing the raw material into the reactor. The amount of HCl added was 20% molar ratio to the amine catalyst.

(3) Results of Verification Experiment 1 FIG. 5 shows the results of Verification Experiment 1 and Comparative Experiment 1 regarding the time until the disproportionation reaction reaches an equilibrium state when the reaction temperature is changed to 50 to 100 ° C. . When the reaction temperature reaches 80 ° C., the time until the disproportionation reaction reaches an equilibrium state is approximately the same in the verification experiment 1 and the comparison experiment 1. In other words, if the reaction temperature is 80 ° C. or higher, catalyst activity equivalent to that in the case of adding HCl can be obtained without performing catalyst reactivation by addition of HCl, and the same reaction rate can be achieved. understood. Therefore, the verification result that the necessity of the regular supply of HCl which is one of the problems to be solved by the present invention is eliminated by setting the reaction temperature to 80 ° C. or higher was obtained.

[Verification experiment 2]
(1) Experimental conditions of verification experiment 2 The case where only a mixture of trichlorosilane and dichlorosilane and dichlorosilane was used as a raw material was verified. The mixing ratio of trichlorosilane and dichlorosilane is a molar ratio of 1: 3. Other experimental conditions were the same as those in the verification experiment 1.

(2) Results of Verification Experiment 2 The results of Verification Experiment 2 are compared with Verification Experiment 1 for the time until the disproportionation reaction reaches an equilibrium state when the reaction temperature is changed to 50 to 100 ° C. It is shown in FIG. Compared with the verification experiment 1, in the verification experiment 2, the time until reaching the equilibrium state was shortened. In addition, the result obtained by using only dichlorosilane as a raw material was almost equal to the result of a mixture of trichlorosilane and dichlorosilane. As already mentioned, the reaction rate of trichlorosilane is slower than that of dichlorosilane or monochlorosilane, so in the coexistence of dichlorosilane, the amine catalyst becomes active and the reaction rate of trichlorosilane is greatly improved. Considered. Therefore, it was found that dichlorosilane and monochlorosilane having a high reaction rate are effective in reactivating the amine catalyst under heating conditions.

[Verification Experiment 3]
Raw materials necessary for producing 1 kg of monosilane, hydrogen chloride to be added, liquid nitrogen for cooling, and catalyst in the case of using this apparatus and in the case of using the conventional technique of adding HCl under the same conditions as in the verification experiment 1 The driving power required for heating for regeneration was compared and verified. The verification results are shown in Table 1. Compared with the prior art, the raw materials trichlorosilane (TCS), HCl and liquid nitrogen could be greatly reduced. Although the driving power increased slightly, a sufficient technical effect was obtained to compensate for the increase in driving power. Moreover, when expensive trichlorosilane is used as a raw material, in addition to the technical effect that the supply amount can be reduced, the economic effect is also great.

1 reaction tower 1a, 3a, 5a, heating means (reboiler)
1b Lower stage (tower bottom)
1c Upper stage (top of tower)
2 Separator 3 Evaporator 4 Feed pump 5 Catalyst regeneration tank 6 Lower cooler 6a Storage tank 7 Control valve

Claims (6)

A reaction column in which monosilane is produced by using hydrogenated silicon chloride as a raw material and a tertiary aliphatic hydrocarbon-substituted amine or / and a hydrochloride of a tertiary aliphatic hydrocarbon-substituted amine as a catalyst, and the reaction column Monosilane is extracted from the reaction product delivered from the upper stage of the reactor, and the separation liquid separated from the condensate composed of other components, and the bottom liquid delivered from the lower stage of the reaction tower are heated, An evaporation tank in which a silicon hydride chloride contained is evaporated to prepare a concentrate, and a part of the raw material or / and a part of the condensate is added to the concentrate and heated to be contained in the concentrate A catalyst regeneration tank in which the catalyst is reactivated and a regeneration solution containing the catalyst is prepared,
An apparatus for producing monosilane, characterized in that a regenerated liquid supplied from the catalyst regeneration tank is supplied to the reaction tower to form a circulation system related to the catalyst.   The catalyst regeneration tank includes a first regeneration tank to which a part of the raw material is supplied and a second regeneration tank to which a part of the condensate is supplied, and the concentrated liquid is formed from the first regeneration tank and the first regeneration tank. 2. The monosilane according to claim 1, wherein after being supplied to one of the regeneration tanks, the liquid supplied from one of the regeneration tanks is further supplied to another regeneration tank to produce a regeneration liquid. manufacturing device.   The separation device is composed of a plurality of stages of separation tanks whose set temperatures are successively lowered, and the reaction product is supplied to the separation tank of the uppermost stream of the highest temperature condition and sequentially transferred to the separation tanks of the next and subsequent stages. And a part of the condensate supplied from each separation tank is supplied to at least one of the catalyst regeneration tank, the evaporation tank, and the reaction tower. The manufacturing apparatus of monosilane of description.   As the lower cooler for cooling the silicon hydride vaporized and delivered from the evaporation tank, a plurality of stages of coolers whose set temperatures are successively lowered are provided and condensed in the first cooler of the uppermost stream stage. As the discharged liquid is taken out, the vapor phase components separated in the first cooler are sequentially transferred to the coolers in the subsequent stages, and the liquid condensed in at least one of the coolers is one of the condensed liquids. The monosilane production apparatus according to claim 1, wherein the monosilane production apparatus is supplied to the catalyst regeneration tank as a part. A monosilane production method, wherein the monosilane is produced by the following steps using the monosilane production apparatus according to claim 1.
(1) Monosilane in the presence of a catalyst comprising a tertiary aliphatic hydrocarbon-substituted amine or / and a tertiary aliphatic hydrocarbon-substituted amine hydrochloride, wherein the raw material hydrogenated silicon chloride is supplied to the reaction tower A reaction product containing
(2) The reaction product delivered from the upper stage of the reaction tower is supplied to a separation device, separated into monosilane and a condensate, and the monosilane is taken out.
(3) The tower bottom liquid supplied from the lower stage of the reaction tower is supplied to the evaporation tank and heated, and the silicon hydride chloride contained in the tower bottom liquid is evaporated to produce a concentrated liquid.
(4) The concentrated liquid is supplied to a catalyst regeneration tank, heated by adding a part of the raw material and / or a part of the condensate separated by the separator, and the catalyst contained in the concentrated liquid Reactivated to produce a regenerating solution,
(5) The regeneration solution is supplied to the reaction tower to form a circulation system related to the catalyst.   At startup, the catalyst and a part of the raw material are supplied to the catalyst regeneration tank, the catalyst is initially activated, and the catalyst liquid and the raw material subjected to the processing are supplied to the reaction tower. The method for producing monosilane according to claim 5, wherein:

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