Microporous molecular separation membrane with high hydrothermal stability
원문보기
IPC분류정보
국가/구분
United States(US) Patent
등록
국제특허분류(IPC7판)
B01D-061/00
B01D-039/00
B01D-029/00
B01D-039/14
출원번호
US-0160992
(2007-01-16)
등록번호
US-8277661
(2012-10-02)
우선권정보
EP-06100388 (2006-01-16)
국제출원번호
PCT/NL2007/050017
(2007-01-16)
§371/§102 date
20081114
(20081114)
국제공개번호
WO2007/081212
(2007-07-19)
발명자
/ 주소
Sah, Ashima
Castricum, Hessel Lennart
Vente, Jaap Ferdinand
Blank, David Hermanus Adrianus
Ten Elshof, Johan Evert
출원인 / 주소
Stichting Energieonderzoek Centrum Nederland
대리인 / 주소
Villacorta, Gilberto M.
인용정보
피인용 횟수 :
13인용 특허 :
9
초록▼
A hydrothermally stable, microporous organic-inorganic hybrid membrane based on silica, having an mean pore diameter of between 0.2 and 1.5 nm, is characterised in that between 5 and 40 mole % of the Si—O—Si bonds have been replaced by moieties having the one of the formulas: Si—{CmH(n-1)X—Si—}q, Si
A hydrothermally stable, microporous organic-inorganic hybrid membrane based on silica, having an mean pore diameter of between 0.2 and 1.5 nm, is characterised in that between 5 and 40 mole % of the Si—O—Si bonds have been replaced by moieties having the one of the formulas: Si—{CmH(n-1)X—Si—}q, Si—CmH(n-2)X2—Si or Si—CmHn—Si{(CmHn)—Si—}y in which m=1-8, n=2m, 2m−2, 2m−4, 2m−6 or 2m−8; provided that n≧2, X=H or (CH2)pSi, p=0 or 1, and q=1, 2, 3 or 4. The membrane can be produced by acid-catalysed hydrolysis of suitable bis-silane precursors such as bis(trialkoxysily)alkanes, preferably in the presence of monoorganyl-silane precursors such as trialkoxy-alkylsilanes.
대표청구항▼
1. A microporous organic-inorganic hybrid membrane based on silica, supported by a mesoporous layer, the microporous membrane having an average pore size of less than 1.5 nm, and in which between a portion of the Si—O—Si bonds have been replaced by moieties having the following formula: Si—CmHn—Si
1. A microporous organic-inorganic hybrid membrane based on silica, supported by a mesoporous layer, the microporous membrane having an average pore size of less than 1.5 nm, and in which between a portion of the Si—O—Si bonds have been replaced by moieties having the following formula: Si—CmHn—Si [I]in a molar ratio represented by the following formulae: Si0.9-1.0M0.0-0.1O1.45-1.55A10.0-0.1A20.45-0.50 [A]or Si0.9-1.0M0.0-0.1O1.45-1.55A10.30-0.36A20.30-0.35 [B]in which:A1 is a monovalent organic moiety of the formula CrHs+1 bound to a silicon atom,A2 is a divalent organic moiety of the formula CmHn bound to two silicon atoms, m=1-8,n=2m, 2m−2, 2m−4, 2m−6, or 2m−8, provided that n≧2, r=1−10,s=2r, 2r−2, 2r−4 or 2r−6, provided that s≧2,M is a metal selected from yttrium, lanthanum, titanium, zirconium, hafnium, aluminum, gallium, germanium and tin. 2. The membrane according to claim 1, in which A1 is methyl. 3. The membrane according to claim 1, in which m=1-3 and n=2m, or m=6 and n=4 or 10. 4. The membrane according to claim 1, which has an average pore diameter between 0.2 and 1.2 nm. 5. The membrane according to claim 1, which shows a stable separation performance in the dehydration of butanol at 150° C. 6. The membrane according to claim 1, which has a thickness of between 20 nm and 2 μm. 7. The membrane according to claim 1, in which the mesoporous layer has been deposited on a macroporous carrier. 8. A method for separating molecules from each other and/or from organic molecules, comprising subjecting the molecules to be separated to a membrane according to claim 1. 9. The method of claim 8, in which the molecules arc hydrogen, nitrogen, ammonia, or water, or a combination thereof. 10. The method of claim 8, in which the organic molecules are alkanes, alkanols, ethers, ketones, or a combination thereof. 11. The membrane according to claim 1, in which m=2. 12. A process of producing a microporous organic-inorganic hybrid membrane, the process comprising: (a) forming a membrane membrane having an average pore size of less than 1.5 nm, and in which a portion of the Si—O—Si bonds have been replaced by moieties having the following formula: Si—CmHn—Si [I]in a molar ratio is represented by the following formula: Si0.9-1.0M0.0-0.1O1.45-1.55A10.0-0.1A20.45-0.50 [A]or Si0.9-1.0M0.0-0.1O1.45-1.55A10.30-0.36A20.30-0.35 [B]in which:A1 is a movement organic moiety of the formula CrHs=1 bound to a silicon atom,A2 is a divalent organic moiety of the formula CmHn bound to two silicon atoms, m=1-8,n=2m, 2m−2, 2m−4, 2m−6, or 2m−8, provided that n≧2, and r=1−10,s=2r, 2r=2, 2r=4 or 2r=6, provided that s≧2,M is a metal selected from yttrium, lanthanum, titanium, zirconium, hafnium, aluminum , gallium, germanium and tin, and(b) supporting the membrane by a mesoporous layer. 13. The process according to claim 12, in which the hydrolysis is carried out using at least 0.8 water molecules per alkoxide group of said silicon and metal alkoxides. 14. The process according to claim 12, in which the hydrolysing is carried out in the absence of a surfactant 15. A microporous organic-inorganic hybrid membrane based on silica supported by a mesoporous layer, the microporous membrane having an average pore size of less than 1.5 nm, and in which between 5 and 24 mole % of the Si—O—Si bonds have been replaced by moieties having one of following formulas: in which:m=1-8,n=2m, 2m−2, 2m−4, 2m−6, or 2m−8, provided that n≧2, andp=0, 1, 2 or 3. 16. A microporous organic-inorganic hybrid membrane based on silica, supported by a mesoporous layer, the microporous membrane having an average pore size of less than 1.5 nm, and in which between 23 and 40% of the Si-O-Si bonds have been replaced by moieties having the following formula: Si—CmHn—Si [I]wherein m=1−8, andn=2m, 2m−2, 2m−4, 2m−6, or 2m−8, provided than n≧2.
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