JP2001039988A - Production of organohalosilane - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a method for producing an organohalosilane through Rochow reaction wherein active metallic silicon particles can be selectively used easily and surely. SOLUTION: This method for producing an organohalosilane comprises reacting metallic silicon particles 10 μm to 10 mm in average size with an organohalide in the presence of a copper catalyst; wherein the metallic silicon particles to be used is such that the surface oxygen level is >=0.05 wt.% and/or >=0.001 g.oxygen/m2.Si surface area as the oxygen concentration difference afforded by analyzing oxygen inside metal for the metallic silicon particles after left to stand in an air atmosphere at 25 deg.C×55%RH for 3 h or longer and small lumps of a metallic silicon material for obtaining the metallic silicon particles through grinding itself. Thereby, active metallic silicon particles in the Rochow reaction can be provided, thus leading to raise the reaction rate, in particular that in activation period and shorten the activation period itself, and improving the accomplishment of the Rochow reaction itself.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

The present invention relates to a Roch (Roch)
ow) A method for producing an organohalosilane by a reaction.

[0002]

2. Description of the Related Art The synthesis of organohalosilanes such as methylchlorosilane is industrially carried out by using a copper catalyst comprising an organic halide such as an alkyl halide or a phenyl halide and metal silicon particles. The reaction is carried out at 250 to 500 ° C. by a so-called Rochow reaction in which a reaction is directly carried out in the presence of a mixed catalyst to which an appropriate promoter has been added. In this reaction, the selectivity of dimethyldichlorosilane, which is the most demanded in the synthesis of methylchlorosilane, should be increased, and in the synthesis of phenylsilane, diphenyldichlorosilane, phenyltrichlorosilane, which is in high demand, can be obtained with a composition that meets the demand. Meanwhile, keeping the reaction speed high is the key technology.

Further, this reaction requires a long time for activation until the reaction reaches a steady state, while the steady state is relatively short, and the activity of the diorganodichlorosilane is reduced by the reduction of the contact activity with time. The yield decreases, for example, in the synthesis of methylsilane, high fractions such as disilane and methyltrichlorosilane due to side reactions increase, and it is necessary to replace the contact body in the reactor. Is also a big problem. Since the Rochow reaction is mainly performed in a fluidized bed or a stirred fluidized bed, various proposals have been made regarding the particle size of metal silicon particles suitable for forming a fluidized bed.

In this reaction, the cost of metal silicon in the raw material cost is high, so that the reaction rate of metal silicon is increased, and at the same time, various types of by-products are usually generated in addition to the main component diorganodichlorosilane. As a by-product, it is important to control the production ratio of this by-product under reaction conditions that are in line with the supply and demand balance of organochlorosilane. This reaction is usually carried out industrially using a reactor such as a fluidized bed, a vibrating fluidized bed, or a stirred fluidized bed in a manner in which a contact body is added to the reaction system. This mechanism is not always clear because it is a very complex gas-solid heterogeneous reaction that occurs at the surface and that the catalyst system is also a solid. And the properties of the metal silicon particles to be used (production area,
It is empirically known that the performance of this reaction is greatly affected by factors such as the manufacturer, the production equipment, and the crushing method) .Several proposals have been submitted, but there is no established theory. In the case of metallic silicon, it is in a state in which a test is performed in advance to determine whether or not this use is possible. As described above, since the metal silicon factors affecting the reaction have not been clarified, this point has been very actively discussed recently in the metal silicon society (for example, Si
silicone forthe Chemical Ind
industry IV: Geiranger, Norwa
y, June 3-5, 1998).

What is important is the reaction activity of the metal silicon particles as a reactant. This has also been studied from various angles, and various proposals have been made (for example, characteristics of the metal silicon itself). Has been made. More specifically, it is already known that aluminum present as an impurity in metallic silicon is effective as a co-catalyst for the Rochow reaction. To be there, H. M.
Rong et al. Suggested that only the active aluminum among the impurities present in the metallic silicon was needed, and suggested a method of measuring it and recommended its use (Procee).
eding Silicon for the Che
medical Industry, p. 69 (199
8)). Japanese Patent Application Laid-Open No. 6-234776 discloses a method for quantifying a dispersion state of an intermetallic compound as an impurity in metal silicon and a selection criterion for controlling reactivity. The lump is cut, the surface is mirror-finished, the form is observed microscopically with a microscope, the structure factor is quantified as a QF value, and the most reactive is to use metal silicon having a value of 18 to 60. It is highly desirable and preferred. Furthermore, there has been proposed a method of adding copper to molten metal silicon and evaluating it based on the form of the used touch body (US Pat. No. 5,281,739).

However, as a result of the present inventors performing these additional tests, it was found that none of them could be distinguished by these methods, but rather that they were all effective only in special limited systems. It could not be adopted as an effective method.

In general, the surface of metal silicon is oxidized and is covered with stable silicon oxide, so that the internal oxidation does not proceed beyond a certain thickness, and the metal silicon is made stable. However, silicon itself has a very high oxidizing property, and it is well known that silicon for semiconductors does not include metal silicon having no oxide film in air. It has been known that the surface of the metal silicon particles for the Rochow reaction has an oxide film to some extent, which affects the Rochow reaction. Regarding the reactivity and selectivity of an oxide film of metal silicon in a methylsilane reaction, G.S. J. Hutch
ing's report (Silicon for the C)
chemical Industry, Geirenge
r, Norway, p. 85-98 (1992)); Laroze's report (Silicon fort)
he Chemical Industry II, L
eon, Norway, p. 121-127 (199
4)), which describes the effect on the reactivity and selectivity of the oxide film. However, these are measured for the metal silicon particles by a local analysis of the oxide film by XPS. Did not mention. Also, J.I. L. Falconer et al. (J. Cata.
l. vol. 159, p. 31-41 (1996))
Discusses the orientation and reactivity of the oxide film and crystal using a silicon wafer, but does not apply to the actual surface of the metal silicon particles for the Rochow reaction, which also mentions the activity of the metal silicon itself. However, the method does not specify metal silicon particles to be used industrially after a measurement method is established.

As described above, the conventionally proposed method is as follows.
It is not necessarily general for industrial use, and when the Rochow reaction is actually performed on metal silicon particles determined by these criteria under conditions where the other factors are completely the same, the results of the reaction vary. It was big. As described above, the conventionally proposed property specification of metal silicon particles can be applied in a special reaction system,
Active metal silicon particles that can be industrially practically used and methods for evaluating the same have been continuously demanded.

The present invention has been made in view of the above circumstances, and it is an object of the present invention to provide a method for producing an organohalosilane in which active metal silicon particles can be easily and reliably selected and used in such a Rochow reaction. Aim.

[0010]

Means for Solving the Problems and Embodiments of the Invention The present inventors have conducted intensive studies to achieve the above object, and as a result, measured the activity of metal silicon particles used in the Rochow reaction as the amount of surface oxygen. The thickness of the oxygen film formed on the surface of the metal silicon to be formed is largely related to the thickness of the oxygen film. In this case, as a method of measuring the amount of surface oxygen, metal silicon particles and pulverization to obtain the metal silicon particles are used. It is effective to separately measure the small mass of the metallic silicon raw material to be measured by the oxygen analysis in metal (inert gas melting furnace oxygen fractionation method) and determine the difference as the surface oxygen content. It is important that the metal silicon particles to be used for the measurement be of a specific type that has been left in an air atmosphere of 25 ° C. × 55% RH for at least 3 hours after the pulverization, so that the activity of the metal silicon particles must be reliably measured. Can It is intended that found made, thus obtained surface oxygen content of 0.05% by weight or more and /
Alternatively, if metal silicon particles having a surface area of 0.001 g · oxygen / m ² · Si or more are selected, it is necessary to directly react an organic halide and metal silicon powder to synthesize a corresponding organohalosilane. It is possible to reliably select metal silicon particles having high activity, shorten the reaction activation time until a steady state called the bite of the reaction of the touch body which was a bottleneck in the reaction, and further reduce the reaction state to the steady state Therefore, even if the reaction rate is increased, the selectivity can be improved, and as a result, the effective utilization rate of silicon can be increased. Although the method was separately used and industrially used after evaluating its reaction activity, it has been found that such a bypass process problem can be solved.

Accordingly, the present invention provides a method for producing a fine powder having an average particle diameter of 10 μm or less.
In a method of producing organohalosilane by reacting 10 mm of metal silicon particles with an organohalide in the presence of a copper catalyst, the metal silicon particles used in this method are 2
Obtained by subjecting metal silicon particles when left in an air atmosphere of 5 ° C. × 55% RH for 3 hours or more and a small lump of a metal silicon raw material for pulverizing and obtaining the metal silicon particles to oxygen analysis in metal. The surface oxygen amount, which is the difference in oxygen concentration, is 0.05% by weight or more and / or 0.001 g · oxygen /
Provided is a method for producing an organohalosilane, characterized by using metal silicon particles having a surface area of not less than m ² · Si.

According to the present invention, a long period of time has conventionally been required in the organochlorosilane synthesis reaction (so-called Rochow reaction) of an alkyl halide such as methyl chloride or an aryl halide such as benzene chloride with a metal catalyst in the presence of a copper catalyst and a cocatalyst. The reduction of the activation time (induction period) to the required steady state and the reaction rate and selectivity of silane formation are important issues, and a method for solving this problem is to improve the catalyst composition and to further reduce the metal silicon particles themselves. Although an improvement was needed, the present invention ensures the optimization of metal silicon particles by elucidating the mechanism of the silane reaction, thereby solving these problems of the Rochow reaction and making a particularly desirable diorgano It is possible to increase the selectivity of dihalosilane, and thus to improve the reaction results. In addition, it is possible to omit a precedent reaction test having a large variation, and it is possible to quantitatively manage the Rochow reaction.

Hereinafter, the present invention will be described in more detail.
In the present invention, an organohalide (organic halide) such as an alkyl halide or an aryl halide is allowed to act on metal silicon particles in the presence of a copper catalyst to obtain a compound represented by the general formula (1): R _m H _n SiX _4-mn (1) (Wherein, R represents an alkyl group having 1 to 4 carbon atoms or an aryl group such as a phenyl group, X represents a halogen atom such as chlorine or bromine, m represents 1, 2 or 3, and n represents 0, 1). Or 2, but m + n is 1, 2 or 3). The present invention relates to metal silicon particles which are a reactant used in a so-called Rochow reaction for synthesizing an organohalosilane represented by the following formula: The time required for activation until the reaction where there was a steady-state reaction, that is, shortening the induction period,
The present invention relates to selection of active metal silicon particles capable of maintaining high activity in a steady state, an activity evaluation method for selection, and use of the particles in a Rochow reaction.

More specifically, metallic silicon is produced by reducing silica together with a carbonaceous material in a high-temperature arc furnace at a temperature of 2500 ° C. or more, and requires a large amount of electric energy and is a material that is inevitably expensive. It is. Therefore, the cost of organohalosilanes, which are precursors of silicone resins made from this material, is dependent on the conversion rate of this expensive metallic silicon to silane (this reaction produces various by-product silanes by side reactions). Therefore, it depends greatly on the production rate (ie, selectivity) of the effective silane in view of the demand balance, and furthermore, the magnitude of the reaction rate which is regarded as important as an industrial process. Therefore, from such a viewpoint, the silicone maker collectively refers to the selectivity and the reaction rate of the product as the reactivity, and demands metal silicon that can exhibit high reactivity with its own manufacturing apparatus. On the other hand, metal silicon manufacturers also use the Rochow reaction and metallic silicon for producing trichlorosilane, which is a semiconductor material similar to the Rochow reaction, because more than half of the total metal silicon consumption is used in these industries. In addition, we actually simulated the reaction and conducted research on the creation of metallic silicon with high reactivity and good selectivity. From the viewpoint of the metallic silicon manufacturer, various amounts of impurities, impurity forms, manufacturing methods, cooling methods, etc. The fact is that we are conducting improvement research from an angle. The results of this research on metallic silicon for chemicals are based on the “Silico International Conference on Metallic Silicon, which is held regularly in Norway once every two years.
n for Chemical Industry ”, and information is exchanged.
The chow reaction itself has not been clearly elucidated, and metal silicon has been evaluated by various companies at present.

The Rochow reaction is a gas-solid heterogeneous reaction between metallic silicon which is a solid at a high temperature and organohalide which is a gas at a high temperature via a catalyst, and its reactivity is a property of metallic silicon as a crystal. Therefore, the method of quantifying the dispersion state of the intermetallic compound, which is an impurity in metallic silicon, which is proposed in Japanese Patent Application Laid-Open No. 6-234776, and the selection criteria for controlling the reactivity are proposed. Makes sense at first glance and is helpful. In this method, the metal silicon block is cut, the surface is mirror-finished,
The surface is microscopically observed with a microscope for a metallurgical morphology, the structure factor is quantified as a QF value, and the use of metallic silicon having a value of 18 to 60 is most highly reactive and preferable. And

However, for ordinary industrial metal silicon,
As a result of analyzing the size of crystallites by the present inventors, it has been found that crystallites of industrial grade metallic silicon are on the order of mm because silicon has high crystallinity. On the other hand, the metal silicon particles actually used for the reaction are at most about 100 μm, which indicates that the metal silicon particles used for the Rochow reaction have several crystallites or less. That is, from these, it was found that the form of the intermetallic compound as an impurity in the metal silicon observed by microscopy does not necessarily represent the crystallinity of the metal silicon which affects the reactivity.

Further, since crystal defects are present in this zone portion, the portion containing the impurities selectively comes out to the surface by pulverization of the metal silicon. M. R
ong et al., Proceeding Silicon f
or the Chemical Industry,
p. 69 (1998) suggests that the aluminum present on the surface of metal silicon particles is active, based on the measurement method (measured by the extraction amount with an aqueous hydrochloric acid solution). Good. However, this part selectively appears on the surface by grinding,
The extraction amount is proportional to the abundance of aluminum, and the extraction rate is almost constant. M. Rong et al. Cannot be applied to the reaction.

As described above, the Rochow reaction is a gas-solid heterogeneous reaction between organohalide which is a gas at a high temperature and metal silicon particles which are a solid at a high temperature. La
roze's report (Silicon for the C)
chemical Industry II, Leon,
Norway, p. 121-127 (1994)). L. Falconer et al. (J. Catal.
vol. 159, p. 31-41 (1996)), it is sufficiently expected that the reactivity greatly depends on the crystal orientation of the metal silicon particles and the surface state of the oxide film and the like. However, J. L. Falcone
A detailed examination of the report by R. et al., in fact, only describes the selectivity and selectivity of metal silicon oxide film in the methylsilane reaction using silicon for semiconductors, and it is impossible to apply it to actual industrial metal silicon particles. There is. In addition, G.
Laroze's report does not clarify the specific measurement method.

Since silicon has high reactivity in air, an oxide film is formed on the surface of metal silicon by contact with air. Generally, the grinding, transport, storage, etc. of the metal silicon lump are performed in an inert gas or an atmosphere with a low oxygen concentration in order to avoid the risk of dust explosion during the grinding, but it is not necessary to completely remove the oxygen. The fact is that an oxide film always exists on the surface. It is also empirically known that the reactivity differs depending on the storage conditions.

On the other hand, in the production process of silicon metal for industrial use,
In order to reduce impurities such as aluminum and calcium, after tapping into a tap container called a ladle, oxygen or air is blown from below in a molten state to remove these impurities as oxides. Although silicon is also slightly oxidized, in this case, the generated silicon monoxide has a high vapor pressure, and as described above, silicon has high crystallinity, so that silicon oxide (silicon monoxide, silicon dioxide)
Is eliminated as slag with the crystal growth by cooling, so that there is almost no oxygen in the metallic silicon.

Accordingly, the present inventors have found that most of the oxygen measured by the inert gas melting furnace oxygen analysis method for metal silicon particles is oxygen present on the surface thereof.
Of course, small particles of slag may be contained inside depending on the manufacturing method, so that confirmation is necessary for analysis.

As a result of the above examinations, the surface oxygen of the metal silicon particles was determined to be higher in the inert gas melting furnace for each of the metal silicon particles and the small lumps (the small lumps of the metal silicon raw material crushed to obtain the particles). Oxygen analyzer (generally referred to as an oxygen analyzer in metal, for example, E
MGA-650) is used to measure the amount of oxygen, the difference is defined as the amount of surface oxygen, and this value is divided by the surface area of the metal silicon particles to calculate the amount of oxygen per unit area. Here, the metal silicon particles to be subjected to such measurement are 25 ° C. × 55% RH.
It has been found that it is important to select metal silicon particles left in the air atmosphere for 3 hours or more. Since the surface oxidation of the metal silicon particles reaches a substantially stable state in 3 hours, the upper limit thereof is not necessarily limited, but it is preferable that the particles be left in the air for 3 to 48 hours, more preferably 16 to 24 hours. .

That is, as described above, the metal silicon particles have a high oxidizing property, and are bonded to oxygen in the air to oxidize the surface. The degree of surface oxidation varies depending on the storage environment and storage time. Therefore, in performing the metal-oxygen analysis of the metal silicon particles in the above “surface oxygen amount”, the value of the metal-oxygen analysis changes depending on what storage state the metal silicon particles were stored, In the present invention, in order to surely know the degree of activity of the metal silicon particles in the Rochow reaction, 25 ° C. × 55
% RH in an air atmosphere of 3 hours or more, preferably 3 to 4 hours.
It is essential to carry out oxygen analysis of the metal silicon particles left for 8 hours, more preferably 16 to 24 hours. In order to obtain metal silicon particles to be subjected to such a measurement, a metal silicon small lump (crushed) is subjected to the size of particles for the Rochow reaction in an inert gas stream or under a low-concentration oxygen atmosphere (15% or less). That is, it can be obtained by a method in which the metal silicon particles are pulverized to an average particle diameter of 10 μm to 10 mm, and the pulverized metal silicon particles are immediately placed in an air atmosphere of 25 ° C. × 55% RH for 3 hours or more, preferably 16 to 24 hours. it can. The measurement of oxygen in metal analysis of the thus obtained metal silicon particles is performed by sample weighing, etc.
In handling at the time of measurement, mounting the sample on the device, and the like, it is not particularly necessary to avoid contact with air. In the present invention, measurement can be performed in any measurement environment.

On the other hand, a small metal silicon lump as another measurement sample is 20 to 100 m from the crushed metal silicon lump.
g small sample is collected, and the small sample is measured as it is. That is, since the metal silicon small lump has a negligible surface area as compared with the pulverized powder, it is not necessary to particularly suppress contact with oxygen.

Then, by calculating this difference, the surface oxygen amount of the metal silicon particles actually subjected to the Rochow reaction is measured.

The feature of the present invention is the selection of metal silicon particles by measuring the amount of oxide film on the surface of the metal silicon particles as described above. A surface oxygen content of 0.05% by weight or more, preferably 0.1% by weight or more, and / or 0.001 g · oxygen / m ² · Si surface area or more by the above measurement;
It has been found that metal silicon particles having a surface area of preferably 0.002 g · oxygen / m ² · Si or more have particularly excellent activity. That is, in this evaluation, the amount of oxygen present on the surface of the metal silicon particles was measured separately for the metal silicon particles and the small lumps thereof by an oxygen-in-metal analysis method (inert gas melting furnace oxygen analysis method). An appropriate method for measuring the amount of oxygen is appropriate.
The one which is left in an air atmosphere at a temperature of 55 ° C. × 55% for 3 hours or more is used, so that it is not necessary to perform a separate reaction test beforehand, and quantitative management becomes possible.

In selecting the metal silicon particles, the higher the surface oxygen content is, the more active it is.
Or less, especially 0.5% by weight or less.

The metal silicon particles actually used for producing the organohalosilane have an average particle diameter of 10 μm to 10 m.
m, satisfying the above selection criteria and stored without surface oxidation (that is, stored in a N ₂ gas atmosphere while avoiding contact with air). It is preferred to use. More preferably, the metal silicon particles (metal silicon particles actually used for the reaction stored without performing such surface oxidation) and a small lump of the metal silicon raw material for obtaining the metal silicon particles by pulverization. Is the difference in oxygen concentration obtained by performing oxygen analysis in metal by the method described above,
% By weight, preferably 0.25% by weight or less, more preferably 0.2% by weight or less, or 0.01% by weight or less.
g · oxygen / m ² · Si surface area or less, preferably 0.00
The surface area is preferably 5 g · oxygen / m ² · Si surface area or less, more preferably less than 0.003 g · oxygen / m ² · Si surface area.

The method for producing an organohalosilane of the present invention can be carried out by using known methods and conditions except that the above-mentioned metal silicon particles are used. For example, as the copper catalyst and the cocatalyst, known ones can be used, and as the organic halide, an alkyl group or an aryl group corresponding to the organohalosilane to be produced, such as methyl chloride, ethyl chloride, or phenyl chloride. In the present invention, for example, an organohalosilane represented by the above formula (1), particularly m =
2,2 = 0 diorganodihalosilane can be produced in high yield.

The amount of the copper catalyst to be added is as follows.
The amount can be 0.1 to 10 parts by weight based on 00 parts by weight. Further, various known cocatalysts can be added to the copper catalyst.

FIG. 1 shows an example of an apparatus for producing an organohalosilane. Reference numeral 1 denotes a fluidized-bed reactor, and a raw material supply tank 3 is connected to a lower part thereof through a raw material supply pipe 2. Metallic silicon and the above-mentioned copper catalyst or a mixed catalyst of a copper catalyst and a co-catalyst are introduced into the lower part of 1. Reference numeral 4 denotes a raw material organic halide tube through which a heater 5 is interposed.
And a gas or vapor of an organic halide is introduced from the bottom of the reactor 1 to form a fluidized bed 1 a of the metal silicon and the catalyst in the reactor 1. In the figure, reference numeral 6 denotes a cooler.

Here, the gas or vapor of the organic halide is preferably introduced at a linear velocity of 2 to 10 cm / sec in a steady state. The reaction is usually 250 to 350
C. can be performed.

The organohalosilane obtained by the reaction is introduced into the first cyclone 8 through a discharge pipe 7 connected to the top of the reactor 1, and after the accompanying solid particles are separated (the solid particles are returned The fluid particles are returned to the fluidized bed 1a through a pipe 9), and the solid particles still entrained in the second cyclone 10 are separated (the solid particles are stored in the separated granular material storage layer 11), and then the first silane condenser 12, Further, the organohalosilane is condensed in the second silane condenser 13 and stored in the silane storage layer 14. The exhaust gas after the solid particles are separated and the organohalosilane is condensed and separated is partly or entirely part of the circulating gas compressor 15.
Is returned to the reactor 1 again through the organic halide return pipe 16 in which is interposed. The return pipe 16 is connected to the raw organic halide pipe 4.

[0034]

According to the present invention, it is possible to provide active metal silicon particles in the Rochow reaction, which leads to a reduction in the reaction rate, particularly the reaction rate in the activation period and the activation period itself. You can improve your own performance. In addition, by doing this, the activity itself of the metal silicon particles can be quantitatively predicted in advance without performing a preliminary test reaction with large variations.
The most suitable metal silicon particles for the Rochow reaction can be selected, and are industrially important and truly revolutionary.

[0035]

The present invention will be described below in more detail with reference to Examples, but the present invention is not limited to the following Examples. In the following examples, parts are parts by weight.

EXAMPLE A steel reactor having a spiral stirrer as shown in FIG. 1 and having a diameter of 8 cm was sufficiently replaced with nitrogen in advance, and the average particle diameter shown in Table 1 was about 50 μm. 100 parts of various kinds of metal silicon particles (different places of production) stored under an inert atmosphere are charged, and nitrogen gas is introduced into the reactor at a linear velocity of 2 cm / sec and flows while being stirred by a spiral stirrer. And heated to 280 ° C. Thereafter, it is a flaky copper foil powder produced by stamping, and has an air-permeable specific surface area of 0.80 m ² / g, an average particle size of 47 μm, a bulk specific gravity of 1.9 g / cm ^{3, and} a flaky copper catalyst. 3 parts of a mixed catalyst obtained by mixing a promoter mainly composed of antimony, brass and bronze were added, and the reaction temperature was increased to 280.
Methyl chloride was gradually added while controlling the temperature to ３００300 ° C. to cause a reaction. Finally, the reaction was continued at a linear speed of 7 cm / sec. When the reaction was continued for 6 hours, the reaction was terminated. Table 2 shows the average silane production rate and the composition of the produced silane during this time.

[0037]

[Table 1]

[0038]

[Table 2]

[Brief description of the drawings]

FIG. 1 is a schematic view showing an example of an apparatus for producing an organohalosilane.

[Explanation of symbols]

 Reference Signs List 1 fluidized bed reactor 1a fluidized bed 2 raw material supply pipe 3 raw material supply tank 4 raw material organic halide pipe 5 heater 6 cooler 7 discharge pipe 8 first cyclone 9 solid particle return pipe 10 second cyclone 11 separated granular material storage Layer 12 First silane condenser 13 Second silane condenser 14 Silane storage layer 15 Circulating gas compressor 16 Organic halide return pipe

 ──────────────────────────────────────────────────続 き Continuing on the front page (72) Inventor Akio Ohori 2-3-1-1, Isobe, Annaka-shi, Gunma Shin-Etsu Kagaku Kogyo Co., Ltd. Gunma Office (72) Inventor Hirofumi Fukuoka 2-chome Isobe, Annaka-shi, Gunma 13-1 Shin-Etsu Kagaku Kogyo Co., Ltd., Gunma Plant (72) Inventor Norio Shinohara 2-13-1, Isobe, Annaka-shi, Gunma Prefecture Shin-Etsu Kagaku Kogyo Co., Ltd. Gunma Plant (72) Inventor Tetsuya Inukai Gunma 2-13-1, Isobe, Annaka-shi Shin-Etsu Chemical Industry Co., Ltd. Gunma Office

Claims (2)

[Claims] 1. A method for producing an organohalosilane by reacting metal silicon particles having an average particle size of 10 μm to 10 mm with an organohalide in the presence of a copper catalyst, wherein the metal silicon particles used in this method are 25 ° C. × 55% RH
The difference between the oxygen concentration obtained by subjecting the metal silicon particles and the small lump of the metal silicon raw material to be pulverized to obtain the metal silicon particles when left in the air atmosphere for 3 hours or more to the oxygen concentration in the metal. Some surface oxygen content is 0.05% by weight
A method for producing an organohalosilane, comprising using metal silicon particles having a surface area of at least 0.001 g · oxygen / m ² · Si. 2. The method according to claim 1, wherein the amount of oxygen adhering to the metal silicon particles used in the method is 0.3% by weight or less.