US4941893A
Expired / Lapsed
US
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Gas separation by semi-permeable membranes
Assignee: Advanced Silicon Materials LLC
•
Filing: 1989-09-19
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Granted: 1990-07-17
•
Expires: 2009-09-19
Abstract
Abstract A method is disclosed for separating gaseous silicon compounds from hydrogen and/or hydracids. Specifically, the method comprises the utilization of semi-permeable membranes for such gaseous separation. Particularly preferred is a composite membrane comprised of a coating separation layer of sulfonated polysulfone and a support layer of polysulfone. Mixtures of hydrogen and silane are particularly suitable for being separated by means of composite membrane separation.
Inventors
- 👤 Shan-Tao Hsieh
- 👤 II George E. Keller
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-11-06 16:10
CPC Classifications
C; C30; C30B; C30B29/00; C30B29/02; C30B29/06; C01; C01B; C01B3/00; C01B3/50; B; B01; B01D; B01D53/00; B01D53/22; B01D53/228; B01D69/00; B01D69/12; B01D69/1213; C01B3/501; C01B3/503; C01B33/00; C01B33/02; C01B33/021; C01B33/027; C01B33/029; C01B33/03; C01B33/035; C01B33/04; C01B33/043; C01B33/08; C01B33/107; C01B33/1071; C01B33/10742; C01B33/10757; C01B33/10763; C01B7/00; C30B25/00; C30B25/02; C01B2203/00; C01B2203/04; C01B2203/0405; C01B2203/0465
Claims Analysis
Total Claims: 79
Claim 1
Independent Claim
138 words
A method for separating at least a first gas selected from the group consisting of H 2 , HX and mixtures thereof contained in a gaseous mixture from at least a second gas selected from the group consisting of SiX a H b and mixtures thereof, where X =a halogen ion, a =0 to 4, b =0 to 4, a +b =4 contained in said gaseous mixture which comprises contacting the gaseous mixture with one surface of a semi-permeable membrane which exhibits selective permeation of the at least first gas over that of the at least second gas, and removing from the vicinity of the opposite surface of the semi-permeable membrane a permeate having a concentration of the at least first gas which is greater than the concentration of the at least first gas in the gaseous mixture.
Claim 2
Independent Claim
138 words
A method for separating at least a first gas selected from the group consisting of H 2 , HX and mixtures thereof contained in a gaseous mixture from at least a second gas selected from the group consisting of SiX a H b and mixtures thereof, where X =a halogen ion, a =0 to 4, b =0 to 4, a +b =4 contained in said gaseous mixture which comprises contacting the gaseous mixture with one surface of a semi-permeable membrane which exhibits selective permeation of the at least first gas over that of the at least second gas, and removing from the vicinity of the opposite surface of the semi-permeable membrane a permeate having a concentration of the at least first gas which is greater than the concentration of the at least first gas in the gaseous mixture.
Claim 3
Dependent Claim
17 words
The method of claim 1, wherein the semi-permeable membrane is an asymmetric membrane or a composite membrane.
Claim 4
Dependent Claim
47 words
The method of claim 2, wherein the composite membrane comprises a porous support layer having substantially no separation characteristics with respect to the gaseous mixture and a substantially non-porous separation layer positioned on the support layer which substantially determines the selective permeation characteristics of the composite membrane.
Claim 5
Dependent Claim
20 words
The method of claim 3, wherein the support layer comprises at least one of polysulfone, polyolefins, polyphenylenesulfide and polyether keytone.
Claim 6
Dependent Claim
11 words
The method of claim 3, wherein the support layer is polysulfone.
Claim 7
Dependent Claim
30 words
The method of claim 3, wherein the separation layer comprises at least one of sulfonated-polysulfone, cellulosic polymers, cellulose acetate, synthetic and natural rubbers, polysiloxanes, polysilazanes, polyesters, polycarbonates, and mixtures thereof.
Claim 8
Dependent Claim
13 words
The method of claim 3, wherein the separation layer is a sulfonated polysulfone.
Claim 9
Dependent Claim
14 words
The method of claim 7, wherein the sulfonated polysulfone is sulfonated bisphenol A polysulfone.
Claim 10
Dependent Claim
22 words
The method of claim 3, wherein the separation layer has a thickness in the range of from about 0.01 to 10.0 microns.
Claim 11
Dependent Claim
22 words
The method of claim 3, wherein the separation layer has a thickness in the range of from about 0.05 to 2.0 microns.
Claim 12
Dependent Claim
18 words
The method of claim 3, wherein the separation layer comprises sulfonated polysulfone and the support layer comprises polysulfone.
Claim 13
Dependent Claim
22 words
The method of claim 3, wherein the separation layer is comprised of cellulose acetate and the support layer is comprised of polysulfone.
Claim 14
Dependent Claim
14 words
The method of claim 3, wherein the support layer is an annealed polymeric material.
Claim 15
Dependent Claim
30 words
The method of claim 2, wherein the asymmetric membrane comprises at least one of sulfonated-polysulfone, cellulosic polymers, cellulose acetate, synthetic and natural rubbers, polysiloxanes, polysilazanes, polyesters, polycarbonates, and mixtures thereof.
Claim 16
Dependent Claim
13 words
The method of claim 2, wherein the asymmetric membrane is a sulfonated polysulfone.
Claim 17
Dependent Claim
14 words
The method of claim 15, wherein the sulfonated polysulfone is sulfonated bisphenol A polysulfone.
Claim 18
Dependent Claim
14 words
The method of claim 1, wherein the composite membrane is in hollow fiber form.
Claim 19
Dependent Claim
23 words
The method of claim 1, wherein the said at least first gas comprises hydrogen and the said at least second gas comprises silane.
Claim 20
Dependent Claim
26 words
The method of claim 1, wherein the said at least first gas is hydrogen chloride and the said at least second gas is trichlorosilane and/or dichlorosilane.
Claim 21
Dependent Claim
19 words
The method of claim 1, wherein HX is hydrogen chloride, hydrogen fluoride, hydrogen bromide, hydrogen iodide, or mixtures thereof.
Claim 22
Dependent Claim
20 words
The method of claim 1, wherein SiX a H b is silicon tetrachloride, trichlorosilane, dichlorosilane, monochlorosilane, silane or mixtures thereof.
Claim 23
Independent Claim
70 words
A method of separating hydrogen from silane contained in a gaseous mixture which comprises contacting the gaseous mixture with one surface of a semi-permeable membrane which exhibits selective permeation for the hydrogen over that of the silane and removing from the vicinity of the opposite surface of the semi permeable membrane a permeate having a concentration of hydrogen which is greater than the hydrogen concentration in the gaseous feed mixture.
Claim 24
Independent Claim
70 words
A method of separating hydrogen from silane contained in a gaseous mixture which comprises contacting the gaseous mixture with one surface of a semi-permeable membrane which exhibits selective permeation for the hydrogen over that of the silane and removing from the vicinity of the opposite surface of the semi permeable membrane a permeate having a concentration of hydrogen which is greater than the hydrogen concentration in the gaseous feed mixture.
Claim 25
Dependent Claim
17 words
The method of claim 22, wherein the semi-permeable membrane is an asymmetric membrane or a composite membrane.
Claim 26
Dependent Claim
47 words
The method of claim 23, wherein the composite membrane comprises a porous support layer having substantially no separation characteristics with respect to the gaseous mixture and a substantially non-porous separation layer positioned on the support layer to substantially determine the selective permeation characteristics of the composite membrane.
Claim 27
Dependent Claim
19 words
The method of claim 24, wherein the separation layer is a sulfonated-polysulfone and the support layer is a polysulfone.
Claim 28
Dependent Claim
19 words
The method of claim 24, wherein the separation layer is cellulose acetate and the support layer is a polysulfone.
Claim 29
Independent Claim
69 words
A method of separating hydrogen from trichlorosilane contained in a gaseous mixture which comprises contacting the gaseous mixture with one surface of a semi-permeable membrane which exhibits selective permeation for the hydrogen over that of the trichlorosilane and removing from the vicinity of the opposite surface of the semi-permeable membrane a permeate having a concentration of hydrogen which is greater than the hydrogen concentration in the gaseous feed mixture.
Claim 30
Independent Claim
69 words
A method of separating hydrogen from trichlorosilane contained in a gaseous mixture which comprises contacting the gaseous mixture with one surface of a semi-permeable membrane which exhibits selective permeation for the hydrogen over that of the trichlorosilane and removing from the vicinity of the opposite surface of the semi-permeable membrane a permeate having a concentration of hydrogen which is greater than the hydrogen concentration in the gaseous feed mixture.
Claim 31
Dependent Claim
17 words
The method of claim 27, wherein the semi-permeable membrane is an asymmetric membrane or a composite membrane.
Claim 32
Dependent Claim
47 words
The method of claim 28, wherein the composite membrane comprises a porous support layer having substantially no separation characteristics with respect to the gaseous mixture and a substantially non-porous separation layer positioned on the support layer to substantially determine the selective permeation characteristics of the composite membrane.
Claim 33
Dependent Claim
19 words
The method of claim 29, wherein the separation layer is a sulfonated-polysulfone and the support layer is a polysulfone.
Claim 34
Dependent Claim
19 words
The method of claim 29, wherein the separation layer is cellulose acetate and the support layer is a polysulfone.
Claim 35
Dependent Claim
144 words
A process for producing a semiconductor silicon metal from a chlorosilane selected from the group consisting of trichlorosilane, dichlorosilane and mixtures thereof, which comprises: (a) providing the chlorosilane in admixture with hydrogen gas in a reaction zone having a temperature sufficient to effect reduction and decomposition of said chlorosilane to silicon metal on a deposition surface; and then (b) contacting exhaust gases leaving the reaction zone comprised of at least unreacted chlorosilanes, hydrogen, and by product hydrogen chloride with a semi-permeable membrane separator which exhibits selective permeation of the hydrogen and hydrogen chloride over the chlorosilanes, to produce a permeate having a concentration of hydrogen and hydrogen chloride which is greater than the concentration of hydrogen and hydrogen chloride in the exhaust gases, and a raffinate having a concentration of chlorosilanes which is greater than the concentration of such chlorosilanes in the exhaust gases.
Claim 36
Dependent Claim
144 words
A process for producing a semiconductor silicon metal from a chlorosilane selected from the group consisting of trichlorosilane, dichlorosilane and mixtures thereof, which comprises: (a) providing the chlorosilane in admixture with hydrogen gas in a reaction zone having a temperature sufficient to effect reduction and decomposition of said chlorosilane to silicon metal on a deposition surface; and then (b) contacting exhaust gases leaving the reaction zone comprised of at least unreacted chlorosilanes, hydrogen, and by product hydrogen chloride with a semi-permeable membrane separator which exhibits selective permeation of the hydrogen and hydrogen chloride over the chlorosilanes, to produce a permeate having a concentration of hydrogen and hydrogen chloride which is greater than the concentration of hydrogen and hydrogen chloride in the exhaust gases, and a raffinate having a concentration of chlorosilanes which is greater than the concentration of such chlorosilanes in the exhaust gases.
Claim 37
Dependent Claim
15 words
The process of claim 32, wherein the raffinate stream is recycled to the reaction zone.
Claim 38
Dependent Claim
31 words
The process of claim 32, wherein the exhaust gases are cooled prior to contacting the membrane separator to a temperature such that a portion of the trichlorosilane is condensed and removed.
Claim 39
Dependent Claim
16 words
The process of claim 32, wherein the semiconductor silicon metal produced is a polycrystalline silicon metal.
Claim 40
Dependent Claim
15 words
The process of claim 32, wherein the semiconductor silicon produced is an epitaxial silicon metal.
Claim 41
Dependent Claim
17 words
The process of claim 32, wherein the semi-permeable membrane is an asymmetric membrane or a composite membrane.
Claim 42
Dependent Claim
47 words
The process of claim 37, wherein the composite membrane comprises a porous support layer having substantially no separation characteristics with respect to the gaseous mixture and a substantially non-porous separation layer positioned on the support layer which substantially determines the selective permeation characteristics of the composite membrane.
Claim 43
Dependent Claim
20 words
The process of claim 38, wherein the support layer comprises at least one of polysulfone, polyolefins, polyphenylenesulfide and polyether ketone.
Claim 44
Dependent Claim
11 words
The process of claim 38, wherein the support layer is polysulfone.
Claim 45
Dependent Claim
30 words
The process of claim 38, wherein the separation layer comprises at least one of sulfonated-polysulfone, cellulosic polymers, cellulose acetate, synthetic and natural rubbers, polysiloxanes, polysilazanes, polyesters, polycarbonates, and mixtures thereof.
Claim 46
Dependent Claim
13 words
The process of claim 38, wherein the separation layer is a sulfonated polysulfone.
Claim 47
Dependent Claim
14 words
The process of claim 42, wherein the sulfonated polysulfone is sulfonated bisphenol A polysulfone.
Claim 48
Dependent Claim
22 words
The process of claim 38, wherein the separation layer has a thickness in the range of from about 0.01 to 10.0 microns.
Claim 49
Dependent Claim
22 words
The process of claim 38, wherein the separation layer has a thickness in the range of from about 0.05 to 2.0 microns.
Claim 50
Dependent Claim
18 words
The process of claim 38, wherein the separation layer comprises sulfonated polysulfone and the support layer comprises polysulfone.
Claim 51
Dependent Claim
22 words
The process of claim 38, wherein the separation layer is comprised of cellulose acetate and the support layer is comprised of polysulfone.
Claim 52
Dependent Claim
14 words
The process of claim 38, wherein the support layer is an annealed polymeric material.
Claim 53
Dependent Claim
30 words
The process of claim 37, wherein the asymmetric membrane comprises at least one of sulfonated-polysulfone, cellulosic polymers, cellulose acetate, synthetic and natural rubbers, polysiloxanes, polysilazanes, polyesters, polycarbonates, and mixtures thereof.
Claim 54
Dependent Claim
13 words
The process of claim 37, wherein the asymmetric membrane is a sulfonated polysulfone.
Claim 55
Dependent Claim
14 words
The process of claim 50, wherein the sulfonated polysulfone is sulfonated bisphenol A polysulfone.
Claim 56
Dependent Claim
14 words
The process of claim 32, wherein the semi-permeable membrane is in hollow fiber form.
Claim 57
Dependent Claim
22 words
The process of claim 32, wherein the reaction zone is a bell-jar reactor and the deposition surface is a stationary elongated rod.
Claim 58
Dependent Claim
24 words
The process of claim 32, wherein the reaction zone is a fluidized bed reactor and the deposition surface is comprised of fluidized seed particles.
Claim 59
Dependent Claim
119 words
A process for producing a semiconductor silicon metal from silane which comprises: (a) providing the silane in admixture with hydrogen gas in a reaction zone having a temperature sufficient to effect reduction and decomposition of said silane to silicon metal on a deposition surface; and then (b) contacting exhaust gases leaving the reaction zone comprised of at least unreacted silane and hydrogen with a semi-permeable membrane separator which exhibits selective permeation of the hydrogen over the silane to produce a permeate having a concentration of hydrogen which is greater than the concentration of hydrogen in the exhaust gases and a raffinate having a concentration of silane which is greater than the concentration of such silane in the exhaust gases.
Claim 60
Dependent Claim
119 words
A process for producing a semiconductor silicon metal from silane which comprises: (a) providing the silane in admixture with hydrogen gas in a reaction zone having a temperature sufficient to effect reduction and decomposition of said silane to silicon metal on a deposition surface; and then (b) contacting exhaust gases leaving the reaction zone comprised of at least unreacted silane and hydrogen with a semi-permeable membrane separator which exhibits selective permeation of the hydrogen over the silane to produce a permeate having a concentration of hydrogen which is greater than the concentration of hydrogen in the exhaust gases and a raffinate having a concentration of silane which is greater than the concentration of such silane in the exhaust gases.
Claim 61
Dependent Claim
14 words
The process of claim 55, wherein the silane is recycled to the reaction zone.
Claim 62
Dependent Claim
17 words
The process of claim 55, wherein the semi-permeable membrane is an asymmetric membrane or a composite membrane.
Claim 63
Dependent Claim
47 words
The process of claim 57, wherein the composite membrane comprises a porous support layer having substantially no separation characteristics with respect to the gaseous mixture and a substantially non-porous separation layer positioned on the support layer which substantially determines the selective permeation characteristics of the composite membrane.
Claim 64
Dependent Claim
20 words
The process of claim 58, wherein the support layer comprises at least one of polysulfone, polyolefins, polyphenylenesulfide and polyether ketone.
Claim 65
Dependent Claim
11 words
The process of claim 58, wherein the support layer is polysulfone.
Claim 66
Dependent Claim
30 words
The process of claim 58, wherein the separation layer comprises at least one of sulfonated-polysulfone, cellulosic polymers, cellulose acetate, synthetic and natural rubbers, polysiloxanes, polysilazanes, polyesters, polycarbonates, and mixtures thereof.
Claim 67
Dependent Claim
13 words
The process of claim 58, wherein the separation layer is a sulfonated polysulfone.
Claim 68
Dependent Claim
14 words
The process of claim 62, wherein the sulfonated polysulfone is sulfonated bisphenol A polysulfone.
Claim 69
Dependent Claim
22 words
The process of claim 58, wherein the separation layer has a thickness in the range of from about 0.01 to 10.0 microns.
Claim 70
Dependent Claim
22 words
The process of claim 58, wherein the separation layer has a thickness in the range of from about 0.05 to 2.0 microns.
Claim 71
Dependent Claim
18 words
The process of claim 58, wherein the separation layer comprises sulfonated polysulfone and the support layer comprises polysulfone.
Claim 72
Dependent Claim
22 words
The process of claim 58, wherein the separation layer is comprised of cellulose acetate and the support layer is comprised of polysulfone.
Claim 73
Dependent Claim
14 words
The process of claim 58, wherein the support layer is an annealed polymeric material.
Claim 74
Dependent Claim
30 words
The process of claim 57, wherein the asymmetric membrane comprises at least one of sulfonated-polysulfone, cellulosic polymers, cellulose acetate, synthetic and natural rubbers, polysiloxanes, polysilazanes, polyesters, polycarbonates, and mixtures thereof.
Claim 75
Dependent Claim
13 words
The process of claim 57, wherein the asymmetric membrane is a sulfonated polysulfone.
Claim 76
Dependent Claim
14 words
The process of claim 70, wherein the sulfonated polysulfone is sulfonated bisphenol A polysulfone.
Claim 77
Dependent Claim
14 words
The process of claim 55, wherein the semi-permeable membrane is in hollow fiber form.
Claim 78
Dependent Claim
22 words
The process of claim 55, wherein the reaction zone is a bell-jar reactor and the deposition surface is a stationary elongated rod.
Claim 79
Dependent Claim
24 words
The process of claim 55, wherein the reaction zone is a fluidized bed reactor and the deposition surface is comprised of fluidized seed particles.
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