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US4462971A
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Preparation of crystalline metal silicate and borosilicate compositions
Assignee: Millennium Petrochemicals Inc
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Filing: 1982-12-29
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Granted: 1984-07-31
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Expires: 2002-12-29
Abstract
Abstract Crystalline metal silicates and metal borosilicate compositions exhibit useful catalytic properties when the reaction mixture from which they are prepared includes a metal whose oxide precipitates at a pH above 7 and an amount of urea or other compound which upon hydrolysis releases ammonia. The precipitated metal hydroxide is incorporated into the crystalline composition as it forms. These compositions exhibit the X-ray pattern of a ZSM-5 zeolite and have an aluminum content of less than 100 wppm and a composition expressed in terms of its oxides as follows: (0.2-80)R(2/n)O: (0.1-20) M(2/m)O: (0-40)B2O3: 100 SiO2:(0-200)H2O where R is tetramethyl ammonium cation, ammonium cation, hydrogen cation, an alkali metal cation, metal cation or mixtures thereof, n is the valence of R, M is a metal whose hydroxide precipitates at a pH above 7 and m is the valence of said metal. These crystalline silicates and borosilicates are usefully employed as catalysts in hydrocarbon conversions.
Inventors
- 👤 James A. Hinnenkamp
- 👤 Vernon V. Walatka, Jr.
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-11-04 13:20
CPC Classifications
C; C01; C01B; C01B35/00; C01B35/08; C01B35/10; C01B35/1009; B; B01; B01J; B01J29/00; B01J29/03; B01J29/035; B01J29/04; Y; Y10; Y10S; Y10S423/00; Y10S423/22
Claims Analysis
Total Claims: 12
Claim 1
Independent Claim
200 words
A method of preparing a crystalline silicate composition which comprises: (a) preparing a first mixture comprising a tetraalkyl ammonium salt, alkali metal hydroxide, silica and water, (b) preparing a second mixture comprising water, a soluble source of a metal whose hydroxide precipitates at a pH above 7 and an amount of urea or a compound which upon hydrolysis releases ammonia, said amount effective to precipitate the hydroxide of said metal, (c) admixing an amount of said first mixture and an amount of said second mixture effective to provide a reaction mixture having an aluminum content of less than about 100 wppm (based on silica) and having a composition in terms of mole ratios of oxides, falling within the following ranges: ______________________________________
OH.sup.- /SiO.sub.2 0.05-3
Q.sup.+ /(Q.sup.+ + A.sup.+)
0.01-1
H.sub.2 O/OH.sup.- 10-800
SiO.sub.2 /M.sub.2/m O
10-10,000
______________________________________ wherein Q + is tetralkyl ammonium ion, A + is alkali metal ion, M is said metal and m is the valence of said metal, whereby the hydroxide of said metal forms a precipitate, (d) maintaining the reaction mixture at a temperature of about 50° to about 250° C. until crystals of metal silicate are formed and (e) separating and recovering said crystals.
Claim 2
Independent Claim
200 words
A method of preparing a crystalline silicate composition which comprises: (a) preparing a first mixture comprising a tetraalkyl ammonium salt, alkali metal hydroxide, silica and water, (b) preparing a second mixture comprising water, a soluble source of a metal whose hydroxide precipitates at a pH above 7 and an amount of urea or a compound which upon hydrolysis releases ammonia, said amount effective to precipitate the hydroxide of said metal, (c) admixing an amount of said first mixture and an amount of said second mixture effective to provide a reaction mixture having an aluminum content of less than about 100 wppm (based on silica) and having a composition in terms of mole ratios of oxides, falling within the following ranges: ______________________________________
OH.sup.- /SiO.sub.2 0.05-3
Q.sup.+ /(Q.sup.+ + A.sup.+)
0.01-1
H.sub.2 O/OH.sup.- 10-800
SiO.sub.2 /M.sub.2/m O
10-10,000
______________________________________ wherein Q + is tetralkyl ammonium ion, A + is alkali metal ion, M is said metal and m is the valence of said metal, whereby the hydroxide of said metal forms a precipitate, (d) maintaining the reaction mixture at a temperature of about 50° to about 250° C. until crystals of metal silicate are formed and (e) separating and recovering said crystals.
Claim 3
Dependent Claim
43 words
A method according to claim 1 wherein a soluble boron compound is admixed with said first mixture and wherein the mole ratios of oxides in said reaction mixture has an additional mole ratio range of SiO 2 /B 2 O 3 : 2-1000.
Claim 4
Dependent Claim
21 words
A method according to claim 1 wherein the metal is iron, cobalt, bismuth, chromium, molybdenum, nickel, tin, platinum or mixtures thereof.
Claim 5
Dependent Claim
28 words
A method according to claim 1 wherein the first mixture of step (a) additionally comprises sulfuric acid and sodium chloride and step (d) is conducted under refluxing conditions.
Claim 6
Independent Claim
208 words
A method of preparing a crystalline silicate composition which comprises: (a) preparing a first mixture comprising a tetraalkyl ammonium salt, alkali metal hydroxide, silica and water, (b) preparing a second mixture comprising water, a soluble source of a metal whose hydroxide precipitates at a pH above 7 and an amount of urea or a compound which upon hydrolysis releases ammonia, said amount effective to precipitate the hydroxide of said metal, (c) maintaining said second mixture under conditions effective to cause the hydroxide of the metal to precipitate, (d) admixing an amount of said first mixture and an amount of said second mixture effective to provide a reaction mixture having an aluminum content of less than about 100 wppm (based on silica) and having a composition in terms of mole ratios of oxides, falling within the following ranges: ______________________________________
OH.sup.- /SiO.sub.2 0.05-3
Q.sup.+ /(Q.sup.+ + A.sup.+)
0.01-1
H.sub.2 O/OH.sup.- 10-800
SiO.sub.2 /M.sub.2/m O
10-10,000
______________________________________ wherein Q + is tetralkyl ammonium ion, A + is alkali metal ion, M is said metal and m is the valence of said metal, (e) maintaining the reaction mixture at a temperature of about 50° to about 250° C. until crystals of metal silicate are formed and (f) separating and recovering said crystals.
Claim 7
Independent Claim
208 words
A method of preparing a crystalline silicate composition which comprises: (a) preparing a first mixture comprising a tetraalkyl ammonium salt, alkali metal hydroxide, silica and water, (b) preparing a second mixture comprising water, a soluble source of a metal whose hydroxide precipitates at a pH above 7 and an amount of urea or a compound which upon hydrolysis releases ammonia, said amount effective to precipitate the hydroxide of said metal, (c) maintaining said second mixture under conditions effective to cause the hydroxide of the metal to precipitate, (d) admixing an amount of said first mixture and an amount of said second mixture effective to provide a reaction mixture having an aluminum content of less than about 100 wppm (based on silica) and having a composition in terms of mole ratios of oxides, falling within the following ranges: ______________________________________
OH.sup.- /SiO.sub.2 0.05-3
Q.sup.+ /(Q.sup.+ + A.sup.+)
0.01-1
H.sub.2 O/OH.sup.- 10-800
SiO.sub.2 /M.sub.2/m O
10-10,000
______________________________________ wherein Q + is tetralkyl ammonium ion, A + is alkali metal ion, M is said metal and m is the valence of said metal, (e) maintaining the reaction mixture at a temperature of about 50° to about 250° C. until crystals of metal silicate are formed and (f) separating and recovering said crystals.
Claim 8
Dependent Claim
43 words
A method according to claim 5 wherein a soluble boron compound is admixed with said first mixture and wherein the mole ratios of oxides in said reaction mixture has an additional mole ratio range of SiO 2 /B 2 O 3 : 2-1000.
Claim 9
Dependent Claim
21 words
A method according to claim 6 wherein the metal is iron, cobalt, bismuth, chromium, molybdenum, nickel, tin platinum or mixtures thereof.
Claim 10
Dependent Claim
30 words
A method according to claim 5 wherein the first mixture of step (a) additionally comprises sulfuric acid and sodium chloride and step (c) and (e) are conducted under refluxing conditions.
Claim 11
Dependent Claim
11 words
A method according to claim 5 wherein the metal is iron.
Claim 12
Dependent Claim
15 words
A method according to claim 9 further containing a boron compound in the first mixture.
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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) | 1987-07-31 | 1988-01-30 | 1988-07-31 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1991-07-31 | 1992-01-30 | 1992-07-31 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 1995-07-31 | 1996-01-30 | 1996-07-31 | $7700.00 | Window Closed / Lapsed |