IP Library Granted Patent US 11,786,877
Granted Patent B2
US 11,786,877 · App. 17/209,835 · Granted Oct 17, 2023

Iron catalyzed hydrochlorination of silicon tetrachloride to trichlorosilane

Inventors: Matthias A. Colomb (Theodore, AL); Bryan H. Nettles (Theodore, AL)
Assignees: Mitsubishi Polycrystalline Silicon America Corporation (MIPSA); HIGH-PURITY SILICON CORPORATION
B01J8/1827B01J8/1872C01B33/10763B01J2208/00938
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Quick Facts
Patent No.
US 11,786,877
App. No.
17/209,835
Granted
Oct 17, 2023
Kind
B2
Abstract

In the hydrochlorination reaction, silicon tetrachloride (STC), metallurgical silicon, and hydrogen are converted to trichlorosilane (TCS) at about 540° C. Previously, a pilot-scale reactor was used to study the yield of TCS produced by the hydrochlorination reaction. The yield observed by experimentation compared favorably with a scalable mathematical model developed to predict the rate of TCS conversion. The model predicted that 90% of the final amount of TCS produced was achieved after the reactant gas traveled a quarter of the vertical distance in the reaction section of the reactor. The pilot-scale reactor was shortened to verify the model predictions. In addition, some catalytic effects on the reaction were studied.

Claims (28)

1. A reactor for producing trichlorosilane (TCS) from the hydrochlorination of silicon tetrachloride (STC) with hydrogen in the presence of metallurgical silicon (Me-Si) comprising:

a reactor vessel comprising:

a distributor plate at the bottom of the inside reactor vessel;

internals inside the vertical length of the reactor vessel with the internals having a high surface area of iron; and

a matrix on the distributor plate with a high surface area of iron to catalyze reactions on the surface of the matrix.

2. The reactor according to claim 1 , wherein the internals include vertically mounted and horizontally supported unfinished surface carbon steel chains.

3. The reactor according to claim 2 , wherein the internals include iron in the form of an iron rich steel or steel alloy selected from the group consisting of: carbon steel, 304 stainless steel and 316 stainless steel.

4. The reactor according to claim 3 , wherein the iron content in steel is greater than about 61 wt %.

5. The reactor according to claim 1 , wherein the matrix is a matrix of carbon steel and stainless steel placed on the distributor plate that allows Me-Si to contact the matrix.

6. The reactor according to claim 1 , wherein the matrix includes iron in the form of an iron rich steel or steel alloy selected from the group consisting of: carbon steel, 304 stainless steel and 316 stainless steel.

7. The reactor according to claim 6 , wherein the iron content in steel is greater than about 61 wt %.

8. The reactor according to claim 1 , wherein the matrix on the distributor plate is iron diffusers with a surface area to volume ratio of about 500 m −1 to about 10,000 m −1 .

9. The reactor according to claim 1 , wherein when silicon is added to the reactor vessel, the iron area in the fluidized bed reactor to silicon weight ratio is between about 0.02-0.15 m 2 /kg.

10. The reactor according to claim 1 , wherein the reactor height is approximately 0.9 to 2.9 meters.

11. A reactor for producing trichlorosilane (TCS) from the hydrochlorination of silicon tetrachloride (STC) with hydrogen in the presence of metallurgical silicon (Me-Si) comprising:

a reactor vessel comprising:

walls formed of steel having at least 61 wt % iron;

a distributor plate at the bottom of the inside reactor vessel;

internals being vertically mounted and horizontally supported unfinished surface carbon steel chains with the internals formed of steel having at least 61 wt % iron; and

a matrix on the distributor plate with iron diffusers with a surface area to volume ratio of 540 to 8583 m −1 and an iron content of at least 61 wt % to catalyze reactions on the surface of the matrix.

12. The reactor according to claim 11 , wherein the reactor height is approximately 0.9 to 2.9 meters.

13. The reactor according to claim 11 , wherein when silicon is added to the reactor vessel, the iron area in the fluidized bed reactor to silicon weight ratio is between about 0.02-0.15 m 2 /kg.

14. A method for producing trichlorosilane (TCS) from the hydrochlorination of silicon tetrachloride (STC) with hydrogen in the presence of metallurgical silicon (Me-Si) comprising:

providing a fluidized bed reactor reaction vessel having internals with a high surface area of iron and having a matrix on a distributor plate with a high surface area of iron to catalyze reactions on the surface of those reactor parts;

introducing metallurgical silicon into the fluidized bed reactor such that the iron area in the fluidized bed reactor to silicon weight ratio is between about 0.02-0.15 m 2 /kg;

introducing hydrogen gas and silicon tetrachloride into the fluidized bed reactor; and

discharging trichlorosilane, the product of a hydrochlorination reaction of silicon tetrachloride, hydrogen, and metallurgical silicon, from the fluidized bed reactor.

15. The method according to claim 14 , wherein when silicon is added to the reactor vessel, the iron area to silicon weight ratio is between about 0.10-0.15 m 2 /kg.

Assignments (3)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 5, 2023
From: MITSUBISHI MATERIALS CORPORATION
To: HIGH-PURITY SILICON CORPORATION
Reel/Frame 063858/0867 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Oct 6, 2021
From: MITSUBISHI POLYCRYSTALLINE SILICON AMERICA CORPORATION (MIPSA)
To: MITSUBISHI POLYCRYSTALLINE SILICON AMERICA CORPORATION (MIPSA); MITSUBISHI MATERIALS CORPORATION
Reel/Frame 057715/0688 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Mar 23, 2021
From: COLOMB, MATTHIAS A.; NETTLES, BRYAN H.
To: MITSUBISHI POLYCRYSTALLINE SILICON AMERICA CORPORATION (MIPSA)
Reel/Frame 055688/0380 →
Continuity (2)
Provisional Application 62993246 · Mar 23, 2020
Related Publication 20210291133A1 · Sep 23, 2021