Claims
- 1. A lamellar mesoporous silica composition containing an electrically neutral gemini amine surfactant in mesopores, the composition having at least one x-ray diffraction peak corresponding to a basal spacing between about 4 and 10 nm and wherein cross-linking of SiO4 tetrahedra to four adjacent silicon sites (Q4) and to three adjacent silicon sites (Q3) corresponds to a Q4/Q3 ratio of at least 5.
- 2. The composition of claim 1 wherein the surfactant is of the formula:
- 3. The composition of claim 1 wherein the surfactant has the formula:
- 4. A lamellar mesoporous silica composition with at least one x-ray diffraction peak corresponding to a basal spacing of between about 4 and 10 nm and wherein cross-linking of the SiO4 tetrahedra of the silica to four adjacent silicon sites (Q4) and to three adjacent silicon sites (Q3) corresponds to a Q4 to Q3 ratio of at least 5.
- 5. The silica composition of claim 4 which is calcined.
- 6. The composition of claim 4 which is thermally stable at 1000° C. and hydrothermally stable at 100° C.
- 7. A lamellar mesoporous silica composition with at least one x-ray diffraction peak corresponding to a basal spacing of between about 4 and 10 nm and wherein cross-linking of the SiO4 tetrahedra sites of the silica to four adjacent silicon sites (Q4) and to three adjacent silicon sites (Q3) corresponds to a Q4 to Q3 ratio of at least 5, and produced from a lamellar silica composition containing a neutral gemini amine surfactant which is removed to produce the lamellar mesoporous silica composition.
- 8. The silica composition of claim 7 which is calcined.
- 9. A mesoporous silica composition containing an electrically neutral gemini amine surfactant in mesopores defining the silica composition.
- 10. The composition of claim 1 wherein a particle morphology is vesicular, bowl shaped, tube-shaped, of an onion layer morphology, or folded ribbon-shaped with a diameter between about 10 and 1400 nm and with a shell thickness between about 2.0 nm and 200 nm, and wherein the shell thickness is comprised of between about 1 and about 50 nanolayers of silica.
- 11. The composition of claim 4 wherein a particle morphology is vesicular, bowl-shaped, tube-shaped, of an onion layer morphology, or folded ribbon-shaped with a diameter between about 10 and 1400 nm and with a shell thickness between about 2.0 nm and 200 nm, and wherein the shell thickness is comprised of between about 1 and about 50 nanolayers of silica composition.
- 12. The composition of claim 4 wherein the composition has the formula MxSi1-xOq when written in anhydrous form where M is an element which forms an oxide, x is between 0.001 and 0.35 and q is between about 1.80 and 2.25.
- 13. A lamellar mesoporous metal oxide and silica composition derived from a silica composition containing an electrically neutral gemini amine surfactant in mesopores, which surfactant has been removed from the silica composition which is then treated with a compound containing one or more functional inorganic elements and then heating the treated silica composition to form the metal oxide and silica composition.
- 14. The composition of claim 13 wherein cross-linking of SiO4 tetrahedra in the silica to four adjacent silicon sites (Q4) and to three adjacent silicon sites (Q3) corresponds to a Q4/Q3 ratio of at least 5.
- 15. The composition of claim 13 with at least one x-ray diffraction line corresponding to a basal spacing of 4 to 10 nm.
- 16. The composition of claim 13 wherein the composition in absence of the surfactant has the anhydrous formula MxSi1-xOq where M is an inorganic element which forms an oxide, x is between about 0.001 and 0.35 and q is between about 1.80 and 2.25.
- 17. The composition of claim 13 wherein the gemini amine surfactant is of the formula:
- 18. The composition of claim 13 wherein the gemini surfactant has the formula:
- 19. The composition of any one of claims 7 or 8 wherein the composition has the formula MxSi1-xOq when written in anhydrous form where M is one or more inorganic elements other than Si which forms an oxide, x is between 0.001 and 0.35 and q is between about 1.80 and 2.25.
- 20. The silica composition of claim 7 which is solvent-extracted to remove the neutral gemini amine surfactant.
- 21. The composition of claim 7 wherein the gemini surfactant is of the formula:
- 22. The composition of claim 7 wherein the gemini amine surfactant has the formula:
- 23. A lamellar mesoporous composition wherein the composition has the formula MxSi1-xOq when written in anhydrous form where M is one or more inorganic elements other than silicon or oxygen, x is between about 0.001 and 0.35, and y is between about 1.80 and 2.25, the composition having at least one x-ray diffraction peak corresponding to a basal spacing between about 4 and 10 nm and wherein cross-linking of SiO4 tetrahedra to four adjacent silicon sites (Q4) and to three adjacent silicon sites (Q3) corresponds to a Q4/Q3 ratio of at least 5.
- 24. The composition of claim 13 wherein a particle morphology is vesicular, bowl-shaped, tube-shaped, of an onion layer morphology, or folded ribbon-shaped with a diameter between about 10 and 1400 nm and with a shell thickness between about 2.0 nm and 200 nm, and wherein the shell thickness is comprised of between about 1 and about 50 nanolayers of silica composition.
- 25. The composition of claim 4 wherein a particle morphology is vesicular, bowl-shaped, tube-shaped, of an onion layer morphology, or folded ribbon-shaped with a diameter between about 10 and 1400 nm and with a shell thickness between about 2.0 nm and 200 nm, and wherein the shell thickness is comprised of between about 1 and about 50 nanolayers of silica composition.
- 26. A lamellar mesoporous metal oxide and silica composition derived from a mixed silica composition and metal oxide forming compound containing an electrically neutral gemini amine surfactant in mesopores, which surfactant has been removed from the silica composition.
- 27. The composition of claim 6 wherein cross-linking of SiO4 tetrahedra in the silica (Q4) and to three adjacent silicon sites (Q3) corresponds to a Q4/Q3 ratio of at least 5.
- 28. The composition of claim 26 wherein the composition has the formula MxSi1-xOq where M is an element which forms an oxide, X is between 0.001 and 0.35 and q is between 1.80 and 2.25.
- 29. The composition of claim 26 with at least one x-ray diffraction line corresponding to a basal spacing of 4 to 10 nm.
- 30. The composition of claim 4 wherein a framework of the silica composition is functionalized by reaction with an organosilane selected from the group consisting of X3SiR, X2SiR2, XSiR3 and mixtures thereof where X is a hydrolyzable moiety and R is an organic moiety which contains an organic functional group.
- 31. The composition of claim 13 wherein the silica composition is functionalized by reaction with an organosilane selected from the group consisting of X3SiR, X2SiR2, XSiR3 and mixtures thereof where X is a hydrolyzable moiety and R is an organic moiety which contains an organic functional group.
- 32. The composition of claim 5 wherein the silica composition is functionalized by reaction with an organosilane selected from the group consisting of X3SiR, X2SiR2, XSiR3 and mixtures thereof where X is a hydrolyzable moiety and R is an organic moiety which contains an organic functional group.
- 33. The composition of any one of claims 4, 5 and 13 wherein a framework of the silica composition is prepared by reacting a silicon alkoxide and a silane of the formula selected from the group consisting of (RO)3SiR1, (RO)2Si(R1)2 and ROSi(R1)3 where R is hydrogen or a lower alkyl group containing 1 to 8 carbon atoms and R1 is selected from the group consisting of hydrogen and an organic moiety.
- 34. A lamellar mesoporous composition wherein the composition has the formulas selected from the group consisting of
- 35. A method for forming a lamellar mesoporous silica composition which comprises:
(a) reacting in a reaction mixture a lower alkyl tetraorthosilicate with a gemini amine surfactant to form the lamellar mesoporous silica composition; and (b) separating the composition from the reaction mixture.
- 36. The method of claim 35 wherein in addition the surfactant is removed from the composition to provide the lamellar mesoporous silica composition.
- 37. The method of claim 36 wherein the surfactant is removed by solvent extraction.
- 38. The method of claim 35 wherein the surfactant is removed by calcination.
- 39. The method of claim 36 wherein the lamellar silica composition is heated with a compound containing a metallic element and then treated to provide a mixed metal or metal oxide and silica composition.
- 40. The method of claim 35 wherein cross-linking of SiO4 tetrahedra of the silica to adjacent silicon sites (Q4) and to three adjacent silicon sites (Q3) corresponds to a Q4/Q3 ratio of SiO4 to SiO3 of at least 5.
- 41. The method of claim 35 wherein the surfactant is of the formula:
- 42. The method of claim 35 wherein the surfactant has the formula:
- 43. The method of claim 35, wherein the composition has at least one x-ray diffraction line corresponding to a basal spacing of about 4 to 10 nm.
GOVERNMENT RIGHTS
[0001] This invention was funded by the National Science Foundation (NSF CHE-96-33798 and CHE-99-03706). The U.S. Government has certain rights in this invention.
Divisions (1)
|
Number |
Date |
Country |
Parent |
09436839 |
Nov 1999 |
US |
Child |
10272636 |
Oct 2002 |
US |