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US4554146A
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Process for preparing a zeolite of the L type using organic templates
Assignee: ExxonMobil Technology and Engineering Co
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Filing: 1983-11-10
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Granted: 1985-11-19
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Expires: 2003-11-10
Abstract
Abstract A zeolite of the L type is prepared by crystallization from a reaction mixture aged at 70 DEG to 260 DEG C. containing water, a source of silica or germania, a source of alumina or gallia, a source of potassium (and optionally up to 40 mole percent of a source of sodium, based on total mole percent of potassium and sodium), and a salt of a tetraalkylammonium cation wherein at least two alkyl groups have more than one carbon atom. Most preferably the cation is tetraethylammonium cation.
Inventors
- 👤 David E. Vaughan
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-10-30 13:10
CPC Classifications
C; C01; C01B; C01B39/00; C01B39/02; C01B39/06; C01B39/065; C01B33/00; C01B33/20; C01B33/26; C01B33/28; C01B33/2807; C01B33/2876; Y; Y10; Y10S; Y10S423/00; Y10S423/28
Claims Analysis
Total Claims: 17
Claim 1
Independent Claim
204 words
A process for synthesizing a crystalline, potassium-containing zeolite having a (Si,Ge)O 2 to (Al,Ga) 2 O 3 ratio of from 3 to 7 and an X-ray powder diffraction pattern which is essentially that given in Table I which comprises: (a) preparing a reaction mixture comprising water, potassium silicate, optionally a source of germania, a source of alumina or gallia, a tetraalkylammonium salt wherein the cation is a tetraethylammonium, tetrapropylammonium, tetrabutylammonium, or bis-(2-hydroxyethyl)dimethylammonium cation, a source of potassium, and up to about 40% by mole fraction of a source of sodium based on total sources of potassium and sodium, said reaction mixtures having a composition, in terms of mole ratios of oxides, within the following ranges: (M,R) 2 O:(Al,Ga) 2 O 3 : 1.4 to 4 (Si,Ge) 2 O:(Al,Ga) 2 O 3 : 2.5 to 15 H 2 O:(Al,Ga) 2 O 3 : 90 to 200 R 2 O:M 2 O: 0.05 to 0.5 where M is K or a mixture of K and Na, and R is the tetraalkylammonium cation; and (b) maintaining the reaction mixture, while it is substantially homogeneous, at between about 70° and 260° C. for between about 1 and 10 days until substantially pure crystals of said zeolite are formed.
Claim 2
Dependent Claim
204 words
A process for synthesizing a crystalline, potassium-containing zeolite having a (Si,Ge)O 2 to (Al,Ga) 2 O 3 ratio of from 3 to 7 and an X-ray powder diffraction pattern which is essentially that given in Table I which comprises: (a) preparing a reaction mixture comprising water, potassium silicate, optionally a source of germania, a source of alumina or gallia, a tetraalkylammonium salt wherein the cation is a tetraethylammonium, tetrapropylammonium, tetrabutylammonium, or bis-(2-hydroxyethyl)dimethylammonium cation, a source of potassium, and up to about 40% by mole fraction of a source of sodium based on total sources of potassium and sodium, said reaction mixtures having a composition, in terms of mole ratios of oxides, within the following ranges: (M,R) 2 O:(Al,Ga) 2 O 3 : 1.4 to 4 (Si,Ge) 2 O:(Al,Ga) 2 O 3 : 2.5 to 15 H 2 O:(Al,Ga) 2 O 3 : 90 to 200 R 2 O:M 2 O: 0.05 to 0.5 where M is K or a mixture of K and Na, and R is the tetraalkylammonium cation; and (b) maintaining the reaction mixture, while it is substantially homogeneous, at between about 70° and 260° C. for between about 1 and 10 days until substantially pure crystals of said zeolite are formed.
Claim 3
Dependent Claim
17 words
The process of claim 1 wherein a source of sodium is not present in the reaction mixture.
Claim 4
Dependent Claim
25 words
The process of claim 1 wherein after step (a) but before step (b) the reaction mixture is blended sufficiently to form a substantially homogeneous mixture.
Claim 5
Dependent Claim
11 words
The process of claim 1 wherein the zeolite crystals are recovered.
Claim 6
Dependent Claim
14 words
The process of claim 1 wherein the source of alumina is kaolin or halloysite.
Claim 7
Dependent Claim
12 words
The process of claim 1 wherein the source of alumina is metakaolin.
Claim 8
Dependent Claim
17 words
The process of claim 1 wherein the reaction mixture is maintained at between 100° and 170° C.
Claim 9
Dependent Claim
13 words
The process of claim 1 wherein the zeolite contains no gallium and germanium.
Claim 10
Dependent Claim
38 words
The process of claim 1 wherein the zeolite has a composition, in terms of mole ratios of oxides, in the range: 1.0 to 1.1(M,R).sub.2 O:Al.sub.2 O.sub.3 :5.2 to 7SiO.sub.2 where M and R are defined in claim 1.
Claim 11
Dependent Claim
38 words
The process of claim 1 wherein the zeolite has a composition, in terms of mole ratios of oxides, in the range: 0.9 to 1.1(M,R).sub.2 O:Al.sub.2 O.sub.3 :2.5 to 5.1SiO.sub.2 where M and R are defined in claim 1.
Claim 12
Dependent Claim
65 words
The process of claim 1 wherein prior to step (b) microcrystals of a zeolite having a composition, in terms of mole ratios of oxides, in the range: 0.9 to 1.3(Na,K).sub.2 O:Al.sub.2 O.sub.3 :5.2 to 6.9SiO.sub.2 :xH.sub.2 O where x is 0 to 9 are added to the blended reaction mixture in an amount of from 0.1 to 10% by weight based on silica and alumina.
Claim 13
Dependent Claim
30 words
The process of claim 1 wherein prior to step (b) the blended reaction mixture is maintained at about 10° to 50° C. for from about 6 hours to 6 days.
Claim 14
Dependent Claim
37 words
The process of claim 1 wherein if the sources of alumina and tetraalkylammonium cation are acid salts, a base is added during step (a) in an effective amount to neutralize the sources of alumina and tetraalkylammonium cation.
Claim 15
Dependent Claim
163 words
A process for synthesizing a crystalline, potassium-containing zeolite having a composition, in terms of mole ratios of oxides, in the range: 1.0 to 1.1(K,R).sub.2 O:Al.sub.2 O.sub.3 :5.2 to 7SiO.sub.2 where R is a tetraethylammonium cation and having an X-ray powder diffraction pattern essentially that given in Table I, which process comprises: (a) preparing a reaction mixture comprising water, potassium silicate, metakaolin, and tetraethylammonium bromide, said reaction mixture having a composition, in terms of mole ratios of oxides, within the following ranges: (K,R) 2 O:Al 2 O 3 : 1.6 to 3.0 SiO 2 :Al 2 O 3 : 4 to 11 H 2 O:Al 2 O 3 : 100 to 160 R 2 O:K 2 O: 0.05 to 0.3 where R is a tetraethylammonium cation; (b) blending the reaction mixture sufficiently to form a substantially homogeneous mixture; and (c) maintaining the blended reaction mixture at between 100° and 170° C. for between 4 and 6 days until crystals of said zeolite are formed.
Claim 16
Dependent Claim
163 words
A process for synthesizing a crystalline, potassium-containing zeolite having a composition, in terms of mole ratios of oxides, in the range: 1.0 to 1.1(K,R).sub.2 O:Al.sub.2 O.sub.3 :5.2 to 7SiO.sub.2 where R is a tetraethylammonium cation and having an X-ray powder diffraction pattern essentially that given in Table I, which process comprises: (a) preparing a reaction mixture comprising water, potassium silicate, metakaolin, and tetraethylammonium bromide, said reaction mixture having a composition, in terms of mole ratios of oxides, within the following ranges: (K,R) 2 O:Al 2 O 3 : 1.6 to 3.0 SiO 2 :Al 2 O 3 : 4 to 11 H 2 O:Al 2 O 3 : 100 to 160 R 2 O:K 2 O: 0.05 to 0.3 where R is a tetraethylammonium cation; (b) blending the reaction mixture sufficiently to form a substantially homogeneous mixture; and (c) maintaining the blended reaction mixture at between 100° and 170° C. for between 4 and 6 days until crystals of said zeolite are formed.
Claim 17
Dependent Claim
44 words
The process of claim 1 additionally comprising the step of washing the substantially pure crystals of said zeolite produced in step (b) at a pH of between 7 and 9 so as to yield a product having a potassium to alumina ratio of 1.0±0.03.
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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) | 1988-11-18 | 1989-05-20 | 1989-11-19 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1992-11-18 | 1993-05-20 | 1993-11-19 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 1996-11-18 | 1997-05-20 | 1997-11-19 | $7700.00 | Window Closed / Lapsed |