US5166111A
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US
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Low-aluminum boron beta zeolite
Assignee: Chevron USA Inc
•
Filing: 1990-10-09
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Granted: 1992-11-24
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Expires: 2010-10-09
Abstract
Abstract A crystalline low-aluminum boron beta zeolite is prepared using a diquaternary ion as a template.
Inventors
- 👤 Stacey I. Zones
- 👤 Dennis L. Holtermann
- 👤 Lawrence W. Jossens
- 👤 Donald S. Santilli
- 👤 Andrew Rainis
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-11-02 04:36
CPC Classifications
C; C10; C10G; C10G47/00; C10G47/02; C10G47/10; C10G47/12; C10G47/16; B; B01; B01J; B01J29/00; B01J29/04; B01J29/86; C01; C01B; C01B35/00; C01B35/08; C01B35/10; C01B35/1009; C01B39/00; C01B39/02; C01B39/06; C01B39/12; C07; C07C; C07C2/00; C07C2/02; C07C2/04; C07C2/06; C07C2/08; C07C2/12; C07C2/54; C07C2/64; C07C2/66; C07C6/00; C07C6/08; C07C6/12; C07C6/126; C10G35/00; C10G35/04; C10G35/06; C10G35/065; C10G45/00; C10G45/58; C10G45/60; C10G45/64; C07C2529/00; C07C2529/86
Claims Analysis
Total Claims: 24
Claim 1
Independent Claim
62 words
A zeolite having a mole ratio of an oxide selected from silicon oxide, germanium oxide, and mixtures thereof to an oxide selected from boron oxide, or mixtures of boron oxide with aluminum oxide, gallium oxide or iron oxide, greater than 10:1 and wherein the amount of aluminum is less than 0.10% by weight and having the X-ray diffraction lines of Table 1(b).
Claim 2
Dependent Claim
62 words
A zeolite having a mole ratio of an oxide selected from silicon oxide, germanium oxide, and mixtures thereof to an oxide selected from boron oxide, or mixtures of boron oxide with aluminum oxide, gallium oxide or iron oxide, greater than 10:1 and wherein the amount of aluminum is less than 0.10% by weight and having the X-ray diffraction lines of Table 1(b).
Claim 3
Dependent Claim
24 words
A zeolite in accordance with claim 1 having a mole ratio of an oxide selected from silicon oxide to boron oxide greater than 100:1.
Claim 4
Dependent Claim
29 words
A zeolite in accordance with claim 1 wherein a portion of the boron in said zeolite is replaced by a first row transition metal or a Group IIIA metal.
Claim 5
Dependent Claim
18 words
A zeolite in accordance with claim 3 wherein the replacing metal is gallium, iron, zinc and mixtures thereof.
Claim 6
Dependent Claim
20 words
A zeolite in accordance with claim 1 wherein a portion of the boron in said zeolite is replaced by silicon.
Claim 7
Dependent Claim
75 words
A zeolite having a composition, as synthesized and in the anhydrous state, in terms of mole ratios of oxides as follows: (1.0 to 5) Q 2 O: (0.1 to 2.0)M 2 O:W 2 O 3 : (greater than 10) YO 2 wherein M is an alkali metal cation, W is boron, Y is selected from silicon, germanium, and mixtures thereof, Q is a diquaternary ammonium ion and having the X-ray diffraction lines of Table 1(a).
Claim 8
Dependent Claim
75 words
A zeolite having a composition, as synthesized and in the anhydrous state, in terms of mole ratios of oxides as follows: (1.0 to 5) Q 2 O: (0.1 to 2.0)M 2 O:W 2 O 3 : (greater than 10) YO 2 wherein M is an alkali metal cation, W is boron, Y is selected from silicon, germanium, and mixtures thereof, Q is a diquaternary ammonium ion and having the X-ray diffraction lines of Table 1(a).
Claim 9
Dependent Claim
21 words
A zeolite in accordance with claim 6 wherein the diquaternary ammonium ion is derived from a compound of the formula: ##STR3##
Claim 10
Dependent Claim
28 words
A zeolite in accordance with claim 1 or 6 which has been ion exchanged with hydrogen, ammonium, rare earth metals, Group IIA metal, or Group VIII metal ions.
Claim 11
Dependent Claim
25 words
A zeolite in accordance with claim 1 or 6 wherein rare earth metals, Group IIA metals, or Group VIII metals are occluded in the zeolite.
Claim 12
Dependent Claim
15 words
A zeolite composition, comprising the zeolite of claim 1 or 6 and an inorganic matrix.
Claim 13
Dependent Claim
21 words
A zeolite in accordance with claim 6 wherein the diquaternary ammonium ion is derived from a compound of the formula: ##STR4##
Claim 14
Dependent Claim
89 words
A zeolite prepared by thermally treating the zeolite, as synthesized and in the anhydrous state, in terms of mole ratios of oxides as follows: (1.0 to 5)Q 2 O:(0.1 to 2.0)M 2 O:W 2 O 3 : (greater than 10) YO 2 wherein M is an alkali metal cation, W is selected from boron, Y is selected from silicon, germanium, and mixtures thereof, Q is a diquaternary ammonium ion and having the X-ray diffraction lines of Table 1(a) and at a temperature from about 200° C. to 820° C.
Claim 15
Dependent Claim
89 words
A zeolite prepared by thermally treating the zeolite, as synthesized and in the anhydrous state, in terms of mole ratios of oxides as follows: (1.0 to 5)Q 2 O:(0.1 to 2.0)M 2 O:W 2 O 3 : (greater than 10) YO 2 wherein M is an alkali metal cation, W is selected from boron, Y is selected from silicon, germanium, and mixtures thereof, Q is a diquaternary ammonium ion and having the X-ray diffraction lines of Table 1(a) and at a temperature from about 200° C. to 820° C.
Claim 16
Independent Claim
207 words
A method for preparing a zeolite having a mole ratio of an oxide selected from silicon oxide, germanium oxide, and mixtures thereof to an oxide selected from boron oxide, or mixtures of boron oxide with aluminum oxide, gallium oxide or iron oxide, greater than 10:1 and wherein the amount of aluminum is less than 0.10% by weight and having the X-ray diffraction lines of Table 1(b), comprising: (a) preparing an aqueous mixture containing sources of a diquaternary ammonium ion wherein the diquaternary ammonium ion is derived from a compound of the formula: ##STR5## an oxide selected from boron oxide, and an oxide selected from silicon oxide, germanium oxide, and mixtures thereof, wherein the reaction mixture has a composition in terms of mole ratios and oxides falling in the ranges: ______________________________________
YO.sub.2 /W.sub.2 O.sub.3
10-200
OH/YO.sub.2 0.10-1.0
Q/YO.sub.2 0.05-0.50
M+/YO.sub.2 0.05-0.30
H.sub.2 O/YO.sub.2
15.300
Q/Q+M+ 0.30-0.90
______________________________________ wherein Y is selected from silicon, germanium, and mixtures thereof, W is boron or mixtures of boron with aluminum, gallium, or iron, Q is a bis(1,4-diAzonia bicyclo[2.2.2]octane) α' ω alkane compound, and M is an alkali metal; (b) maintaining the mixture at a temperature of at least 140° C. until the crystals of said zeolite form; and (c) recovering said crystals.
Claim 17
Independent Claim
207 words
A method for preparing a zeolite having a mole ratio of an oxide selected from silicon oxide, germanium oxide, and mixtures thereof to an oxide selected from boron oxide, or mixtures of boron oxide with aluminum oxide, gallium oxide or iron oxide, greater than 10:1 and wherein the amount of aluminum is less than 0.10% by weight and having the X-ray diffraction lines of Table 1(b), comprising: (a) preparing an aqueous mixture containing sources of a diquaternary ammonium ion wherein the diquaternary ammonium ion is derived from a compound of the formula: ##STR5## an oxide selected from boron oxide, and an oxide selected from silicon oxide, germanium oxide, and mixtures thereof, wherein the reaction mixture has a composition in terms of mole ratios and oxides falling in the ranges: ______________________________________
YO.sub.2 /W.sub.2 O.sub.3
10-200
OH/YO.sub.2 0.10-1.0
Q/YO.sub.2 0.05-0.50
M+/YO.sub.2 0.05-0.30
H.sub.2 O/YO.sub.2
15.300
Q/Q+M+ 0.30-0.90
______________________________________ wherein Y is selected from silicon, germanium, and mixtures thereof, W is boron or mixtures of boron with aluminum, gallium, or iron, Q is a bis(1,4-diAzonia bicyclo[2.2.2]octane) α' ω alkane compound, and M is an alkali metal; (b) maintaining the mixture at a temperature of at least 140° C. until the crystals of said zeolite form; and (c) recovering said crystals.
Claim 18
Dependent Claim
67 words
A method in accordance with claim 13 wherein the aqueous mixture has a composition in terms of mole ratios of oxides falling in the ranges: YO 2 /W 2 O 3 , greater than 10; Q/YO 2 , 0.05:1 to 0.50:1; wherein Y is selected from silicon, germanium, and mixtures thereof, W is selected from boron, and Q is a bis(1-diAzonia bicyclo [2.2.2]octane) α' ω alkane compound.
Claim 19
Dependent Claim
21 words
A method in accordance with claim 13 wherein the diquaternary ammonium ion is derived from a compound of the formula: ##STR6##
Claim 20
Dependent Claim
77 words
The method of claim 13 wherein the reaction mixture has a composition in terms of mole ratios and oxides falling in the ranges: ______________________________________
YO.sub.2 /W.sub.2 O.sub.3
30-100
OH/YO.sub.2
0.25-0.50
Q/YO.sub.2
0.25-0.35
M+/YO.sub.2
0.05-0.10
H.sub.2 O/YO.sub.2
25-60
Q/Q+M+ 0.60-0.80
______________________________________ wherein Y is selected from silicon, germanium, and mixtures thereof, W is boron or mixtures of boron with aluminum, gallium, or iron, Q is a bis(1,4-diAzonia bicyclo[2.2.2]octane) α' ω alkane compound, and M is an alkali metal.
Claim 21
Independent Claim
208 words
A method for preparing a zeolite having a mole ratio of an oxide selected from silicon oxide, germanium oxide, and mixtures thereof to an oxide selected from boron oxide, or mixtures of boron oxide with aluminum oxide, gallium oxide or iron oxide, greater than 10:1 and wherein the amount of aluminum is less than 0.10% by weight and having the X-ray diffraction lines of Table 1(b), comprising: (a) preparing an aqueous mixture containing sources of a diquaternary ammonium ion wherein the diquaternary ammonium ion is derived from a compound of the formula: ##STR7## an oxide selected from boron oxide, and an oxide selected from the silicon oxide, germanium oxide, and mixtures thereof, wherein the reaction mixture has a composition in terms of mole ratios and oxides falling in the ranges: ______________________________________
YO.sub.2 /W.sub.2 O.sub.3
10-200
OH/YO.sub.2 0.10-1.0
Q/YO.sub.2 0.05-0.50
M+/YO.sub.2 0.05-0.30
H.sub.2 O/YO.sub.2
15.300
Q/Q+M+ 0.30-0.90
______________________________________ wherein Y is selected from silicon, germanium, and mixtures thereof, W is boron or mixtures of boron with aluminum, gallium, or iron, Q is a bis(1,4-diAzonia bicyclo[2.2.2]octane) α' ω alkane compound, and M is an alkali metal; (b) maintaining the mixture at a temperature of at least 140° C. until the crystals of said zeolite form; and (c) recovering said crystals.
Claim 22
Independent Claim
208 words
A method for preparing a zeolite having a mole ratio of an oxide selected from silicon oxide, germanium oxide, and mixtures thereof to an oxide selected from boron oxide, or mixtures of boron oxide with aluminum oxide, gallium oxide or iron oxide, greater than 10:1 and wherein the amount of aluminum is less than 0.10% by weight and having the X-ray diffraction lines of Table 1(b), comprising: (a) preparing an aqueous mixture containing sources of a diquaternary ammonium ion wherein the diquaternary ammonium ion is derived from a compound of the formula: ##STR7## an oxide selected from boron oxide, and an oxide selected from the silicon oxide, germanium oxide, and mixtures thereof, wherein the reaction mixture has a composition in terms of mole ratios and oxides falling in the ranges: ______________________________________
YO.sub.2 /W.sub.2 O.sub.3
10-200
OH/YO.sub.2 0.10-1.0
Q/YO.sub.2 0.05-0.50
M+/YO.sub.2 0.05-0.30
H.sub.2 O/YO.sub.2
15.300
Q/Q+M+ 0.30-0.90
______________________________________ wherein Y is selected from silicon, germanium, and mixtures thereof, W is boron or mixtures of boron with aluminum, gallium, or iron, Q is a bis(1,4-diAzonia bicyclo[2.2.2]octane) α' ω alkane compound, and M is an alkali metal; (b) maintaining the mixture at a temperature of at least 140° C. until the crystals of said zeolite form; and (c) recovering said crystals.
Claim 23
Dependent Claim
207 words
A zeolite having a mole ratio of an oxide selected from silicon oxide, germanium oxide, and mixtures thereof to an oxide selected from boron oxide, or mixtures of boron oxide with aluminum oxide, gallium oxide or iron oxide, greater than 10:1 and wherein the amount of aluminum is less than 0.10% by weight and having the X-ray diffraction lines of Table 1(b), prepared by a method comprising: (a) preparing an aqueous mixture containing sources of a diquaternary ammonium ion wherein the diquaternary ammonium ion is derived from a compound of the formula: ##STR8## an oxide selected from boron oxide, and an oxide selected from silicon oxide, germanium oxide, and mixtures thereof, wherein the reaction mixture has a composition in terms of mole ratios and oxides falling in the ranges: ______________________________________
YO.sub.2 /W.sub.2 O.sub.3
10-200
OH/YO.sub.2 0.10-1.0
Q/YO.sub.2 0.05-0.50
M+/YO.sub.2 0.05-0.30
H.sub.2 O/YO.sub.2
15.300
Q/Q+M+ 0.30-0.90
______________________________________ wherein Y is selected from silicon, germanium, and mixtures thereof, W is boron or mixtures of boron with aluminum, gallium, or iron, Q is a bis(1,4-diAzonia bicyclo[2.2.2]octane) α' ω alkane compound, and M is an alkali metal; (b) maintaining the mixture at a temperature of at least 140° C. until the crystals of said zeolite form; and (c) recovering said crystals.
Claim 24
Dependent Claim
207 words
A zeolite having a mole ratio of an oxide selected from silicon oxide, germanium oxide, and mixtures thereof to an oxide selected from boron oxide, or mixtures of boron oxide with aluminum oxide, gallium oxide or iron oxide, greater than 10:1 and wherein the amount of aluminum is less than 0.10% by weight and having the X-ray diffraction lines of Table 1(b), prepared by a method comprising: (a) preparing an aqueous mixture containing sources of a diquaternary ammonium ion wherein the diquaternary ammonium ion is derived from a compound of the formula: ##STR8## an oxide selected from boron oxide, and an oxide selected from silicon oxide, germanium oxide, and mixtures thereof, wherein the reaction mixture has a composition in terms of mole ratios and oxides falling in the ranges: ______________________________________
YO.sub.2 /W.sub.2 O.sub.3
10-200
OH/YO.sub.2 0.10-1.0
Q/YO.sub.2 0.05-0.50
M+/YO.sub.2 0.05-0.30
H.sub.2 O/YO.sub.2
15.300
Q/Q+M+ 0.30-0.90
______________________________________ wherein Y is selected from silicon, germanium, and mixtures thereof, W is boron or mixtures of boron with aluminum, gallium, or iron, Q is a bis(1,4-diAzonia bicyclo[2.2.2]octane) α' ω alkane compound, and M is an alkali metal; (b) maintaining the mixture at a temperature of at least 140° C. until the crystals of said zeolite form; and (c) recovering said crystals.
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USPTO Annuity & Maintenance Windows
| Annuity Stage | Window Opens | Payment Deadline | Surcharge Period Until | Estimated Fee | Status |
|---|---|---|---|---|---|
| 3.5 Years (Year 4) | 1995-11-24 | 1996-05-25 | 1996-11-24 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1999-11-24 | 2000-05-25 | 2000-11-24 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 2003-11-24 | 2004-05-25 | 2004-11-24 | $7700.00 | Window Closed / Lapsed |