WO2016091240A1

WO2016091240A1 - Method for recovering hexachlorodisilane from chlorosilane mixtures in process offgas streams

Info

Publication number: WO2016091240A1
Application number: PCT/DE2015/000562
Authority: WO
Inventors: Michael Schley; Martin Katz; Friedrich Schaaff
Original assignee: Silicon Products Bitterfeld Gmbh & Co. Kg
Priority date: 2014-12-10
Filing date: 2015-11-20
Publication date: 2016-06-16
Also published as: CN107207267A; KR20170091623A; DE102014018435A1; EP3230206A1

Abstract

The invention pertains to a method for recovering hexachlorodisilane from mixtures, present within process offgas streams, of chorosilanes of the general formula Si_xH_yCl_2x+2-y, where x = 1 and y = 0 - 3 and x = 2 and y = 0 - 5. The problem addressed by the present invention is therefore that of providing a method to allow high-yield isolation of the hexachlorodisilane from the aforesaid chlorosilane mixtures arising in the thermal reaction of hydrogen with monosilanes of the general formula Si_xH_yCl_2x+2-y, where x is 1 and y is 0 - 2. The problem is solved by a method for recovering hexachlorodisilane from mixtures, present within process offgas streams, of chorosilanes of the general formula Si_xH_yCl_2x+2-y, where x = 1 and y = 0 - 3 and x = 2 and y = 0 - 5, which is characterized in that the offgas streams or fractions thereof are converted to the liquid phase and then the partially hydrogenated chlorodisilanes of the general formula Si_xH_yCl_2x-2y-1 (x = 2, y = 1 - 5) that are in the chlorosilane mixture are additionally reacted catalytically to hexachlorodisilane, which is isolated from the resulting mixture by distillation.

Description

Process for recovering hexachlorodisilane from mixtures of chlorosilanes contained in process effluent streams

The invention relates to a process for recovering hexachlorodisilane from mixtures of chlorosilanes having the general formula Si _x H _y Cl _{2x + 2} y contained in process exhaust gas streams, where x = 1 and y = 0-3 and x = 2 and y = 0-5 is.

In addition to chlorodisilanes having the general formula Si _x H _y Cl _{X + 2} - _y , where x = 1 and y = 0-3, the process exhaust streams can also significant proportions of partially hydrogenated chlorodisilanes having the general formula SixHyCI _{2X + 2} y, where x = 2 and y = 1-5, and small proportions of higher boiling silicon compounds and in the

Reaction with hydrogen Chlorosilanes of the general formula Si _x H _y Cl ₂ X _{+ 2} .y, where x = 1 and y = 0 - 2 are included.

Processes such as the chemical vapor deposition of silicon

Monosilanes, having the general formula Si _x HyCl _{2X + 2} - _yi where x = 1 and y = 0 -

2, as in the chemical vapor deposition of the

Siemens process as well as other CVD processes of microelectronics using chlorosilanes, the hydrogenation of silicon tetrachloride to produce trichlorosilane or the trichlorosilane synthesis of metallurgical silicon, for example, produce such process gases.

In addition, such exhaust gases also occur in the case of plasma reactions (T> 200 ° C.) of chlorosilanes, with the general formula Si _x H _y Cl 2 x ₊ 2 _-y where x = 1 and y = 1 -

3 is without hydrogen being added. Processes like heating of

Trichlorosilane in an electrode burner at> 200 ° C, as in DE1 42848B

described, can supply these process exhaust gases.

In the industrially customary process steps known per se, the low-boiling components are used in one or more distillation steps

(Boiling temperatures <57 ° C at 1013.25 mbar) of the said process gases partially or completely separated. The distillation sump remains

Chlorosilane mixture with components having a boiling point> 57 ° C (b ei 1013.25 mbar). This chlorosilane mixture contains Si ₂ Cl ₆ (hexachlorodisilane) and further partially hydrogenated chlorodisilanes having the general formula

Si _x H _y _{Cl 2} X _{+ 2-} y, where x is 2 and y is 1-5. Hexachlorodisilane is an important starting material in microelectronics. The compound is, inter alia, precursor in CVD deposition for high-purity silicon nitride, silicon oxide or silicon carbide layers. Continues to play

Hexachlorodisilane plays an important role in transistor fabrication in memory chips. Low-temperature epitaxy becomes epitaxial silicon layers

deposited.

So far, the difficulty was due to the very similar boiling points of hexachlorodisilane and other partially hydrogenated chlorodisilanes a pure fraction of hexachlorodisilane (S ^ C ^) to win. For this purpose, an energetically and technically complicated distillation with a high number of separation stages is required, as described in EP 1264798. The resulting yields of hexachlorodisilane are low and can only be increased by the chlorination of the partially hydrogenated chlorosilanes by an additional chlorination step with the chlorinating agent chlorine. The use of chlorine increases the equipment and safety costs.

Previous procedures aimed in particular to destroy the chlorodisilanes having the general formula Si _x HyCl ₂ x _{+ 2-y} , where x is 2 and y is 0-5, which usually occur as undesirable by-products in the process. The pure hydrolysis of these components disadvantageously led to highly reactive solids. For this reason, the destruction of this designed

high-boiling components difficult. Destruction of these chlorosilanes is described in EP 2544795 B1 and US 2009/0104100 A1.

Another method describes the reaction with chlorine gas, which leads, according to EP 2036859 B1, to cleavage of the silicon-silicon bond and thus the high-quality disilanes having the general formula Si _x HyCl ₂ x _{+ 2} y, where x is 2 and y equal to 1-5 is to be destroyed. The aim of this reaction is to convert the disilane to silicon tetrachloride and return it back to the material cycle in order to increase the material yield.

In DE 3503262 A1, the catalytic conversion of hexachlorodisilane /

Pentachlorodisilane mixtures of organotitrogen or phosphorus compounds described. The objective of the applicants is complete decomposition of the listed disilanes to trichlorosilane, silicon tetrachloride and solid polychlorosilane. The present invention is therefore based on the object to provide a method which is a separation of Hexachlordisilans with high yields from the described chlorosilane mixtures, which in the thermal reaction of hydrogen with monosilanes of the general formula Si _x HyCl ₂ x + 2-y, where x equals 1 and y equals 0 - 2, is available.

The object is achieved by a method for obtaining

Hexachlorodisilane from mixtures of process gases contained in

Chlorosilanes with the general formula SixHyCl ₂ x + 2-y. where x = 1 and y = 0 - 3 and x = 2 and y = 0 - 5, which is characterized in that the exhaust gas streams or fractions thereof are converted into the liquid phase and then the partially hydrated chlorodisilanes contained in the mixture of chlorosilanes general formula Si _x H _y Cl 2x-2 -i (x = 2, y = 1-5) are reacted catalytically in addition to hexachlorodisilane and separated from the resulting mixture hexachlorodisilane by distillation.

Advantageous developments are specified in the subclaims.

Thereafter, the transfer of the exhaust gases into the liquid phase takes place by condensation or absorption in a solvent and the catalytic reaction is carried out at a temperature of 0 to 100 ° C and a pressure up to 20 bar.

In an advantageous embodiment of the invention, the reaction is carried out in a batch or in a continuous process.

A further advantageous embodiment of the method is that the catalyst to inorganic, such as Al ₂ 0 ₃ , Si0 ₂ or organic, such as co-polymer of styrene and divinylbenzene, solids immobilized, dispersed or in a mixture of

Chlorosilanes dissolved is used.

An inventive embodiment provides that as catalysts following

Connections are used:

primary, secondary, tertiary amines of general formula I:

where R 1, R 2 and R 3 are hydrogen, alkyl with Ci to Ci ₀ , cycloalkyl with a ring size of 4 to 8, alkenyl with Ci to Ci ₀ or aryl with a ring size of 4 to 8, groups and R1 * R 2 R 3, R 1 = R 2 R 3 or R 1 = R 2 = R 3, where the organic radicals may be linear or branched,

Quaternary amines / ammonium salts of general formula II:

where R ₁ , R 2, R 3 and R 4 are hydrogen, alkyl with Ci to Ci ₀ , cycloalkyl with a ring size of 4 to 8, alkenyl with Ci to C ₁₀ or aryl with a ring size of 4 to 8 groups and A halides , Pseudohalogenide, phosphates and sulfates and R1 * R2 * R3 * R4, R1 = R2 = R3 * R4 or R1 = R2 * R3 * R4 or R1 = R2 = R3 = R4, where the organic radicals may be linear or branched , heterocyclic nitrogen compounds of general formula III:

(III) with a ring size of 4 to 8,

where R ₁ , R 2, R 3 and R 4 are hydrogen, alkyl with Ci to Ci ₀ , cycloalkyl with a ring size of 4 to 8, alkenyl with Ci to Ci ₀ or aryl with a ring size of 4 to 8 groups and R1 R2 R3 R4, R1 = R2 = R3 * R4 or R1 = R2 * R3 R4 or R1 = R2 = R3 = R4, where the organic radicals may be linear or branched, heterocyclic aromatic compounds (azines) having one to four nitrogen - Atoms in the ring, such as pyridine, pyrazine, triazine and their derivatives, their radicals hydrogen, alkyl with Ci to Ci ₀ , Cycloalkyl- with a ring size of 4 to 8, Alkenyl- with Ci to C ₁₀ or aryl- with a Ringröße may be from 4 to 8 groups, wherein the organic radicals may be linear or branched.

- Organophosphorus compounds, such as primary, secondary, tertiary phosphines, the general formula IV

wherein R 1, R 2 and R 3 are hydrogen, alkyl with Ci to C ₁₀ , cycloalkyl having a ring size of 4 to 8, alkenyl with Ci to C1 ₀ or aryl with a ring size of 4 to 8 groups and R 1 R 2 R 3 , R 1 = R 2 * R 3 or R 1 = R 2 = R 3, where the organic radicals may be linear or branched,

and

, Quaternary phosphines of the general formula V

wherein R1, R2, R3 and R4 are hydrogen, alkyl with d to Ci ₀ , cycloalkyl having a ring size of 4 to 8, alkenyl with Ci to C1 ₀ or aryl with a ring size of 4 to 8 groups and A halides , Pseudohalogenide, phosphates and sulfates and R1 R2 # R3 * R4, R1 = R2 = R3 * R4 or R1 = R2 R3 * R4 or R1 = R2 = R3 = R4, wherein the organic radicals may be linear or branched.

In one development of the invention, the chlorosilane mixture is mixed with silicon tetrachloride, which advantageously leads to an increase in yield.

A further embodiment is characterized in that after the catalytic conversion of the chlorosilane mixture, the distillative separation of the

Reaction mixture takes place or the catalytic reaction takes place during a reactive distillation. The advantages here are in particular the lower equipment costs and the better energy balance. Increase the temperature, then catalytically

Implementing and distilling immediately is energetically and technologically more advantageous than increasing the temperature, catalytically converting, cooling, reheating and then distilling.

Particularly advantageous catalysts such as alkylated or arylated tertiary amines such as trimethylamine, in homogeneous form or immobilized on inorganic or organic support materials alkylated or arylated tertiary amines are used which have groupings such as dimethylamino groups, heterocyclic nitrogen compounds (azines), pyridine groups or nitriles or quaternary amines, with trimethylammonium chloride groups on one

organic carrier material, such as e.g. a copolymer of styrene and divinylbenzene or on an inorganic support material, e.g. Silica, are immobilized.

The heterogeneous catalyst is used in the form of pellets containing a

Particle size greater than 0.5 mm. A fine fraction is not included. The catalyst still has sufficient stability at at least 100 ° C., is insoluble and substantially does not tend to split off the amine. The catalytically active functional groups are easily accessible.

For the homogeneous reaction, tertiary alkylamines, such as:

Trimethylamine, which are soluble in the system one and have a significantly lower boiling point than that of hexachlorodisilane, so that a good separation is guaranteed.

According to the invention, chlorosilane mixtures having proportions of chlorosilanes of the general formula Si _x HyCl _{2X + 2} .y, where x is 2 and y is 0-5, of

Process exhaust gas streams from the reaction of hydrogen with chlorosilanes having the general formula Si _x HyCl ₂ x + 2-y, where x is 1 and y is 0-2 processed. The aim of this processing is the extraction of high-boiling

Components SixHyCl ₂ x + 2-y, where x> 1 (boiling point> 100 ° C, at 1013.25 mbar), in particular hexachlorodisilane (Si ₂ Cl ₆ ).

The catalytic conversion of the chlorosilane mixture leads mainly to the formation of hexachlorodisilane and higher boiling silicon compounds, which a particularly clean separation of Hexachlordisilan allows.

The boiling point differences which can advantageously be achieved with the invention are so serious in the system obtained that separation of the components can take place with little technical and energy expenditure. Consequently, the purity of the obtained fractions can be increased. In contrast to EP 1264798 A1 here is a complete implementation of all partially hydrogenated

Chlorodisilanes. In addition, according to the invention by the catalytic

Implementation advantageously formed additional hexachlorodisilane and thus increases the overall yield.

Further advantages of the present invention are that hexachlorodisilane can be separated from the exhaust gases of the processes described with low equipment costs and low costs, without additional safety risks, in high purity. This is achieved by means of the selective catalytic reaction of partially hydrogenated chlorodisilane moieties in the chlorosilane mixture, having the general formula Si _x HyCl ₂ x _{+ 2} -y- where x is 2 and y is 0-5.

By means of the catalytic reaction, the yield of hexachlorodisilane is considerably increased.

The invention will be described with reference to Figure 1, in which in a flow chart

inventive method is shown schematically, and explained in more detail in subsequent embodiments.

According to flow chart Fig.1 are in the process for the production of

Hexachlorodisilane from mixtures of chlorosilanes in a process exhaust gas 1 process exhaust gases, after conversion into the liquid phase by

Condensation in a distillative pre-separation 2 separated into a separation region 3 and a separation region 4.

In the separation region 3 here predominantly chlorosilanes of the general formula Si _x H _y Cl2x + 2-y, (x = 1, y = 0 - 3) collect and in the separation region 4, a mixture of SiCU with proportions between 10 and 99% by mass and Si _x H _y Cl 2 _x + 2-y (x = 2, y = 0 - 5) with proportions between 1 and 90 mass%.

The further treatment of the mixture of chlorosilanes, in the separation area 4 obtained, with the aim in particular to enrich and separate hexachlorodisilane.

According to the invention, in an advantageous variant of the method

catalytic conversion 5 of the chlorosilane mixture from the separation region 4 performed. The resulting as a result of the catalytic reaction 5

The reaction mixture is then separated in a distillative separation 7 into three fractions. A fraction 7.1 contains chlorosilanes of the general formula Si _x HyCl ₂ x-2y-i (x = 1, y = 0 - 2). It is a separation of the monosilanes contained for the return to the process cycle conceivable. A fraction 7.2 contains the target product hexachlorodisilane Si ₂ Cl ₆ and the distillation bottom 7.3 contains a mixture of higher-boiling silicon compounds having> 2 silicon atoms in the

Molecule.

In a further advantageous variant of the method according to the invention, the chlorosilane mixture from the separation region 4 is catalytically reacted during the distillation by means of a reactive distillation 6. After separation of fraction 6.1, which contains mainly trichlorosilane, the catalyst must be separated from the liquid phase prior to further distillation in order then to obtain silicon tetrachloride as a separate fraction 6.2 and hexachlorodisilane as fraction 6.3. A distillation bottoms 6.4 remains from higher-boiling silicon compounds having> 2 silicon atoms in the molecule.

Embodiment 1 (Comparative Example)

767.0 g of a chlorosilane mixture, which corresponds to the high boiler fraction of a distillation of exhaust gases of a silicon production, were separated by distillation. Fractions listed below were obtained. The swamp was not investigated further.

Table 1. Overview of the composition of the starting mixture and of the fractions of the comparative example (TCS = trichlorosilane, STC = silicon tetrachloride, TCDS = tetrachlorodisilane, PCDS = pentachlorodisilane, HCDS = hexachlorodisilane) Masses in g

description

Total TCS STC TCDS PCDS HCDS

Chlorosilane before the

788.2 13.0 508.7 0.8 88.9 176.7 Distillation

1st fraction (boiling range up to

507.8 12.7 495.1

120 ° C)

2nd fraction (boiling range 120 -

31, 6 0.8 27.3 3.6 130 ° C)

3rd fraction (boiling range 130 -

97.0 56.440 40.6 140 ° C)

4th fraction (boiling range 140 -

44.6 2.8 41, 8 140 ° C)

5th fraction (boiling point 144.8 ° C) 86.1 86.1

Swamp 21, 1

Exemplary embodiment 2 (according to FIG. 1, implementation 5)

In a three-necked flask, 303.3 g of chlorosilane mixture with 0.4 g of the

Catalyst Amberlyst A21 ^{® added} at 20 ° C. After one week, the composition was redetermined (Table 2). The catalyst was filtered off and the mixture was separated by distillation. Three fractions were taken. The third fraction or the bottoms contained, in addition to hexachlorodisilane, further higher-boiling silicon compounds.

Table 2. Overview of compositions of the mixtures and the fractions of Example 1 (TCS = trichlorosilane, STC = silicon tetrachloride, TCDS =

Tetrachlorodisilane, PCDS = pentachlorodisilane, HCDS = hexachlorodisilane and HSS = higher boiling silicon compounds). Composition determined by NMR spectroscopy. Masses in g

description

Total TCS STC TCDS PCDS HCDS HSS

chlorosilane

before catalytic 303.3 5.5 212.8 0.8 33.8 50.4

implementation

chlorosilane

after catalytic 303.3 23.6 224.3 53.3 2.1

implementation

1st faction

(Boiling range up to 140 219.1 27.0 192.1

° C)

2nd faction

55.3 53.4 1, 9 (boiling point 140 ° C)

3. Swamp 28.9 0.9 28.0

Embodiment 3 (according to FIG. 1, implementation 5)

In a three necked flask, 20.5 g of Amberlyst A21 ^® (ca. 900 mL) chlorosilane mixture at 20 ° C and 1352.3 g. The mixture was analyzed by NMR spectroscopy after one week. The catalyst was filtered off and the mixture was separated by distillation. It was possible to obtain 232.7 g of hexachlorodisilane (Table 3).

Table 3. Overview of Compositions of the Mixtures of Example 2 (TCS = trichlorosilane, STC = silicon tetrachloride, TCDS = tetrachlorodisilane, PCDS logo CNRS logo INIST

Pentachlorodisilane, HCDS = hexachlorodisilane and HSS = higher boiling

Silicon compounds). Composition determined by NMR spectroscopy.

Masses in g

description

Total TCS STC TCDS PCDS HCDS HSS

chlorosilane

before catalytic 1352.3 24.3 949.3 3.3 150.9 224.5

implementation

chlorosilane

after catalytic 1352.3 122.9 983.1 232.7 13.6

implementation Exemplary embodiment 4 (according to FIG. 1, reactive distillation 6)

In a distillation apparatus 1344.6 g of a Chlorsilangemischs were added to 19.9 g of the catalyst Amberlyst A21 ^® and heated to 45 ° C. Here, 119.9 g of trichlorosilane were separated. Subsequently, the catalyst was filtered off. 851.7 g of silicon tetrachloride and 236.8 g of hexachlorodisilane were subsequently separated by distillation from the remaining solution. The bottom remained as a yellowish solution (136.2 g). This solution contained an additional 4.0 g of hexachlorodisilane (NMR spectroscopic analysis). The rest became higher boiling

Silicon compounds assigned (Table 4).

Table 4. Overview of compositions of the mixtures and the fractions of Example 1 (TCS = trichlorosilane, STC = silicon tetrachloride, TCDS =

Tetrachlorodisilane, PCDS = pentachlorodisilane, HCDS = hexachlorodisilane and HSS = higher boiling silicon compounds). Composition determined by NMR spectroscopy.

Masses in g

description

Total TCS STC TCDS PCDS HCDS HSS

High-boiling mixture

before reactive 1344.6 24.2 943.8 3.2 150.1 223.3

distillation

1st fraction 119.9 119.9

2. Fraction 851, 7 851.7

3rd fraction 236.8 236.8

Swamp 136,2 4,2 132

Exemplary embodiment 5 (according to FIG. 1, implementation 5)

In a three-necked flask, 304 g of chlorosilane mixture with 0.4 g of a

Dimethylamino-functionalized silica (catalyst) at 20 ° C was added. After stirring for one week at room temperature, the composition became again determined (Table 5). The catalyst was filtered off and the mixture was separated by distillation. Three fractions were taken. The third fraction or the bottom contained lordisilan next Hexach further higher-boiling silicon compounds.

Table 5. Overview of Compositions of the Mixtures and of the Fractions of Example 4 (TCS = trichlorosilane, STC = silicon tetrachloride, TCDS logo CNRS logo INIST

Masses in g

description

Total TCS STC TCDS PCDS HCDS HSS

chlorosilane

before catalytic 304.0 5.6 214.4 0.8 33.4 49.8

implementation

Chlorosilane after

304.0 23.9 223.8 54.1 2.2 catalytic conversion

1st fraction (boiling range

219.1 27.2 191, 9

up to 1 0 ° C)

2nd fraction (boiling point

54.6 54.4 0.2 140 ° C)

3. bottom 30.3 0.8 29.5

Exemplary embodiment 6 (according to FIG. 1, implementation 5)

In a three-necked flask, 305.2 g of chlorosilane mixture were mixed with 0.4 g of a pyridine-functionalized silica (catalyst) at 20 ° C. After one week at room temperature, the composition was redetermined (Table 6). The catalyst was filtered off and the mixture was separated by distillation. Three fractions were taken. The third fraction or sump contained beside

Hexachlorodisilane further higher-boiling silicon compounds.

Table 6. Overview of Compositions of the Mixtures and the Fractions of Example 5 (TCS = trichlorosilane, STC = silicon tetrachloride, TCDS = tetra- chlorodisilane, PCDS = pentachlorodisilane, HCDS = hexachlorodisilane and HSS = higher boiling silicon compounds). Composition determined by NMR spectroscopy.

Masses in g

description

Total TCS STC TCDS PCDS HCDS HSS

chlorosilane

before catalytic 305.2 5.5 215.1 0.8 33.8 50.0

implementation

Chlorosilane after

305.2 21.7 224.2 56.2 3.1 catalytic conversion

1st fraction (boiling range

218,2 26,9 191, 3

up to 140 ° C)

2nd fraction (boiling point

56.9 56.8 0.1 140 X)

3. Swamp 30.1 0.5 29.6

Exemplary embodiment 7 (according to FIG. 1, implementation 5)

In a three-necked flask, 298.4 g of chlorosilane mixture with 0.4 g of a

Diphenylphosphine-functionalized silica (catalyst) at 20 ° C After one week at room temperature, the composition was redetermined (Table 7). The catalyst was filtered off and the mixture was separated by distillation. Three fractions were taken. The third fraction or the bottom contained, in addition to hexachlorodisilane, further higher-boiling silicon compounds. Table 7. Overview of compositions of the mixtures and of the fractions of Example 6 (TCS = trichlorosilane, STC = silicon tetrachloride, TCDS = tetrachlorodisilane, PCDS = pentachlorodisilane, HCDS = hexachlorodisilane and HSS = higher-boiling silicon compounds). Composition determined by NMR spectroscopy.

Masses in g

description

Total TCS STC TCDS PCDS HCDS HSS

chlorosilane

before catalytic 298.4 3.9 213.1 0.4 31, 4 49.6

implementation

Chlorosilane after

298.4 24.1 219.1 52.1 3.1 catalytic conversion

1st fraction (boiling range

214.7 23.4 191, 3

up to 140 ° C)

2nd fraction (boiling point

54.3 53.2 0.1 140 ° C)

3. Swamp 29.4 0.5 28.9

LIST OF REFERENCE NUMBERS

1 process exhaust area

2 pre-separation (distillative)

3 separation area

4 separation area

5 implementation

6 reactive distillation

6.1 Fraction

6.2 Fraction

6.3 Fraction

6.4 distillation bottoms

7 distillation

7.1 Fraction

7.2 fraction

7.3 distillation bottoms

Claims

claims

1. A process for recovering hexachlorodisilane from mixtures of chlorosilanes having the general formula Si _x HyCl _{2X + 2-} y, where x = 1 and y = 0-3 and x = 2 and y = 0-5, in process exhaust streams,

characterized in that

the exhaust gas streams or fractions thereof are transferred into the liquid phase and then the partially hydrogenated chlorodisilanes of the general formula SixHyCl 2 _X- 2y-i (x = 2, y = 1-5) present in the mixture of the chlorosilanes, in addition to catalytically

Hexachlorodisilane be reacted and from the resulting mixture

Hexachlorodisilane is separated by distillation.

2. The method according to claim 1,

characterized in that

the conversion of the exhaust gases into the liquid phase by condensation or

Absorption takes place in a solvent and the catalytic reaction is carried out at a temperature of 0 to 100 ° C and a pressure up to 20 bar.

3. The method according to claim 1 or 2,

characterized in that

the implementation is carried out in batch or in a continuous process.

4. The method according to any one of claims 1 to 3,

characterized in that

the catalyst is used on inorganic, such as Al ₂ 0 ₃ , Si0 ₂ or organic, such as copolymer of styrene and divinylbenzene, solids immobilized, dispersed or dissolved in a mixture of chlorosilanes.

5. The method according to any one of claims 1 to 4,

characterized in that

be used as catalysts primary, secondary, tertiary amines of the general formula I.

wherein R1, R2 and R3 are hydrogen, alkyl with Ci to C1 ₀ , cycloalkyl having a ring size of 4 to 8, alkenyl with Ci to Ci ₀ or aryl with a ring size of 4 to 8, groups and R1 R2 # R3, R1 = R2 # R3 or R1 = R2 = R3, where the organic radicals may be linear or branched,

Quaternary amines / ammonium salts of the general formula II

where R ₁ , R 2, R 3 and R 4 are hydrogen, alkyl with Ci to Ci ₀ , Cycloalkyl- with a ring size of 4 to 8, Alkenyl- with Ci to Ci ₀ or Aryl- with a ring size of 4 to 8 groups and A halides , Pseudohalides, phosphates and sulfates and R 1 is R 2 * R 3 * R 4, R 1 = R 2 = R 3 R 4 or R 1 = R 2 * R 3 * R 4 or R 1 = R 2 = R 3 = R 4, where the organic radicals may be linear or branched,

- Heterocyclic nitrogen compounds of general formula III

having a ring size of 4 to 8, wherein R1, R2, R3 and R4 are hydrogen, alkyl with Ci to C10, cycloalkyl having a ring size of 4 to 8, alkenyl with Ci to C ₁₀ or aryl with a ring size of 4 to 8 groups are and R1 R2 R3 ^ R4,

R1 = R2 = R3 * R4 or R1 = R2 R3 * R4 or R1 = R2 = R3 = R4, where the

organic radicals may be linear or branched, Heterocyclic aromatic compounds (azines) having one to four nitrogen atoms in the ring, such as pyridine, pyrazine, triazine and their derivatives, their radicals hydrogen, alkyl with Ci to C1 ₀ , cycloalkyl with a ring size of 4 to 8, alkenyl - With Ci to C ₁₀ or aryl can be with a ring size of 4 to 8 groups, wherein the organic radicals may be linear or branched.

Organophosphorus compounds, such as primary, secondary, tertiary phosphines, of the general formula IV

where R ₁ , R 2 and R 3 are hydrogen, alkyl with Ci to Ci ₀ , cycloalkyl with a ring size of 4 to 8, alkenyl with Ci to C ₁₀ or aryl with a ring size of 4 to 8 groups and R1 * R2 * R 3, R 1 = R 2 * R 3 or R 1 = R 2 = R 3, where the organic radicals may be linear or branched,

and

, Quaternary phosphines of the general formula V

where R 1, R 2, R 3 and R 4 are hydrogen, alkyl with C 1 to C ₁₀ , cycloalkyl having a ring size of 4 to 8, alkenyl with C 1 to C ₁₀ or aryl having a ring size of 4 to 8 groups and A halides , Pseudohalogenide, phosphates and sulfates and R1 * R2 * R3 R4, R1 = R2 = R3 * R4 or R1 = R29 R3 * R4 or R1 = R2 = R3 = R4, wherein the organic radicals may be linear or branched.

6. The method according to any one of claims 1 to 5,

characterized in that

the chlorosilane mixed with silicon tetrachloride.

7. The method according to any one of claims 1 to 6,

characterized in that

after the catalytic conversion of the chlorosilane mixture, the distillative separation (7) of the reaction mixture is carried out or the catalytic reaction takes place during a reactive distillation (6).