Method for manufacturing synthetic mesoporous crystalline material

Claim 3

The method of claim 1 wherein R comprises cetyltrimethylammonium, octadecyltrimethylammonium, benzyltrimethylammonium, cetylpyridinium, myristyltrimethylammonium, decyltrimethylammonium, dodecyltrimethylammonium or dimethyldidodecylammonium.

Claim 4

The method of claim 1 wherein said organic directing agent comprises cetyltrimethylammonium hydroxide.

Claim 5

The method of claim 1 further comprising compositing said recovered composition of matter with a binder prior to contacting said recovered composition of matter with steam at elevated temperature.

Claim 6

The method of claim 4 wherein said binder is inert.

Claim 7

The method of claim 4 wherein said binder comprises alumina.

Claim 8

The method of claim 1 further comprising contacting said recovered composition of matter with an ammonium-containing compound prior to contacting said recovered composition of matter with steam.

Claim 9

The method of claim 7 wherein said ammonium-containing compound is NH 4 NO 3 .

Claim 10

The method of claim 1 wherein said steam contacting step (iv) is conducted at temperature above 220° F.

Claim 11

The method of claim 9 wherein said steam contacting step (iv) is conducted at temperature above 300° F.

Claim 12

The method of claim 10 wherein said steam contacting step (iv) is conducted at temperatures of from about 300° F. to about 900° F.

Claim 13

The method of claim 1 wherein said steam contacting step (iv) is conducted at pressures from about 0.1 to about 10 Bar.

Claim 14

The method of claim 1 further comprising contacting said recovered composition of matter with steam at elevated temperature for from about 5 minutes to about 24 hours.

Claim 15

The method of claim 1 wherein said reaction mixture has a composition, in terms of mole ratios, within the following ranges: ______________________________________ X.sub.2 O.sub.3 /YO.sub.2 0 to 0.5 Al.sub.2 O.sub.3 /SiO.sub.2 0 to 0.01 X.sub.2 O.sub.3 /(YO.sub.2 + Z.sub.2 O.sub.5) 0.1 to 100 X.sub.2 O.sub.3 /(YO.sub.2 + W'O + Z.sub.2 O.sub.5) 0.1 to 100 Solvent/ 1 to 1500 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) OH.sup.- /YO.sub.2 0 to 10 (M.sub.2/e O + R.sub.2/f O)/ 0.01 to 20 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) M.sub.2/e O/ 0 to 10 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) R.sub.2/f O/ 0.01 to 2.0 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) ______________________________________ wherein M is said alkali or alkaline earth metal cation, W' is said divalent element, X is said trivalent element, Y is said tetravalent element, Z is said pentavalent element, R is said organic directing agent, and e and f are the weighted average valences of M and R, respectively.

Claim 16

The method of claim 14 wherein R comprises cetyltrimethylammonium, octadecyltrimethylammonium, benzyltrimethylammonium, cetylpyridinium, myristyltrimethylammonium, decyltrimethylammonium, dodecyltrimethylammonium or dimethyldidodecylammonium.

Claim 17

The method of claim 14 wherein said organic directing agent comprises cetyltrimethylammonium hydroxide.

Claim 18

The method of claim 14 further comprising compositing said recovered composition of matter with a binder prior to contacting said recovered composition of matter with steam at elevated temperature.

Claim 19

The method of claim 1 wherein said reaction mixture has a composition, in terms of mole ratios, within the following ranges: ______________________________________ X.sub.2 O.sub.3 /YO.sub.2 0 to 0.5 X.sub.2 O.sub.3 /(YO.sub.2 + Z.sub.2 O.sub.5) 01 to 100 X.sub.2 O.sub.3 /(YO.sub.2 + W'O + Z.sub.2 O.sub.5) 0.1 to 100 Solvent/ 1 to 1500 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) OH.sup.- /YO.sub.2 0 to 10 (M.sub.2/e O + R.sub.2/f O)/ 0.01 to 20 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) M.sub.2/e O/ 0 to 10 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) R.sub.2/f O/ 0.01 to 2.0 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) ______________________________________ wherein M is said alkali or alkaline earth metal cation, W' is said divalent element, X is said trivalent element, Y is said tetravalent element, Z is said pentavalent element, R comprises a mixture of component (a) an ion of the formula R 1 R 2 R 3 R 4 Q+, wherein Q is nitrogen or phosphorus and wherein at least one of R 1 , R 2 , R 3 and R 4 is aryl or alkyl of from 6 to about 36 carbon atoms or combinations thereof, the remainder of R 1 , R 2 , R 3 and R 4 being selected from the group consisting of hydrogen, alkyl of from 1 to 5 carbon atoms and combinations thereof, and component (b) an additional ion of the formula R 1 R 2 R 3 R 4 Q+ wherein R 1 , R 2 , R 3 and R 4 are selected from the group consisting of hydrogen, alkyl of 1 to 5 carbon atoms and combinations thereof, and wherein e and f are the weighted average valences of M and R, respectively.

Claim 20

The method of claim 18 wherein R comprises cetyltrimethylammonium, octadecyltrimethylammonium, benzyltrimethylammonium, cetylpyridinium, myristyltrimethylammonium, decyltrimethylammonium, dodecyltrimethylammonium or dimethyldidodecylammonium,

Claim 21

The method of claim 18 wherein said organic directing agent comprises cetyltrimethylammonium hydroxide.

Claim 22

The method of claim 18 further comprising compositing said recovered composition of matter with a binder prior to contacting said recovered composition of matter with steam at elevated temperature.

Claim 23

The method of claim 21 wherein said binder is inert.

Claim 24

The method of claim 21 wherein said binder comprises alumina.

Claim 25

The method of claim 1 wherein said reaction mixture has a composition, in terms of mole ratios, within the following ranges: ______________________________________ Al.sub.2 O.sub.3 /SiO.sub.2 0 to 0.1 Solvent/SiO.sub.2 1 to 1500 OH.sup.- /SiO.sub.2 0 to 10 (M.sub.2/e O + R.sub.2/f O)/ 0.01 to 20 (SiO.sub.2 + Al.sub.2 O.sub.3) M.sub.2/e O/ 0 to 5 (SiO.sub.2 + Al.sub.2 O.sub.3) R.sub.2/f O/ 0.01 to 2 (SiO.sub.2 + Al.sub.2 O.sub.3) ______________________________________ wherein M is said alkali or alkaline earth metal cation, R is said organic directing agent, e and f are the weighted average valences of M and R, respectively.

Claim 26

The method of claim 24 wherein R comprises cetyltrimethylammonium, octadecyltrimethylammonium, benzyltrimethylammonium, cetylpyridinium, myristyltrimethylammonium, decyltrimethylammonium, dodecyltrimethylammonium or dimethyldidodecylammonium.

Claim 27

The method of claim 24 wherein said organic directing agent comprises cetyltrimethylammonium hydroxide.

Claim 28

The method of claim 25 wherein said source of an oxide of silicon comprises an organic silicate.

Claim 29

The method of claim 27 wherein said organic silicate comprises a quaternary ammonium silicate.

Claim 30

The method of claim 27 wherein said organic silicate comprises tetraethylorthosilicate.

Claim 31

The method of claim 24 further comprising compositing said recovered composition of matter with a binder prior to contacting said recovered composition of matter with steam at elevated temperature.

Claim 32

The method of claim 30 wherein said binder is inert.

Claim 33

The method of claim 30 wherein said binder comprises alumina.

Claim 34

The method of claim 1 wherein said crystalline phase has, after calcination, a hexagonal arrangement of uniformly-sized pores having diameters of at least about 13 Angstrom Units and exhibits a hexagonal electron diffraction pattern than can be indexed with a d 100 value greater than about 18 Angstrom Units.

Claim 35

The method of claim 33 wherein R comprises cetyltrimethylammonium, octadecyltrimethylammonium, benzyltrimethylammonium, cetylpyridinium, myristyltrimethylammonium, decyltrimethylammonium, dodecyltrimethylammonium or dimethyldidodecylammonium,

Claim 36

The method of claim 34 wherein said organic directing agent comprises cetyltrimethylammonium hydroxide.

Claim 37

The method of claim 33 further comprising compositing said recovered composition of matter with a binder prior to contacting said recovered composition of matter with team at elevated temperature.

Claim 38

The method of claim 36 wherein said binder is inert.

Claim 39

The method of claim 36 wherein said binder comprises alumina.

Claim 40

The method of claim 33 wherein said reaction mixture has a composition, in terms of mole ratios, within the following ranges: ______________________________________ X.sub.2 O.sub.3 /YO.sub.2 0 to 0.5 Al.sub.2 O.sub.3 /SiO.sub.2 0 to 0.01 X.sub.2 O.sub.3 /(YO.sub.2 + Z.sub.2 O.sub.5) 0.1 to 100 X.sub.2 O.sub.3 /(YO.sub.2 + W'O + Z.sub.2 O.sub.5) 0.1 to 100 Solvent/ (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) 1 to 1500 OH.sup.- /YO.sub.2 0 to 10 (M.sub.2/e O + R.sub.2/f O)/ 0.01 to 20 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) M.sub.2/e O/ 0 to 10 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) R.sub.2/f O/ 0.01 to 2.0 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) ______________________________________ wherein M is said alkali or alkaline earth metal cation, W' is said divalent element, X is said trivalent element, Y is said tetravalent element, Z is said pentavalent element, R is said organic directing agent, and e and f are the weighted average valences of M and R, respectively.

Claim 41

The method of claim 33 wherein said reaction mixture has a composition, in terms of mole ratios, within the following ranges: ______________________________________ X.sub.2 O.sub.3 /YO.sub.2 0 to 0.5 X.sub.2 O.sub.3 /(YO.sub.2 + Z.sub.2 O.sub.5 0.1 to 100 X.sub.2 O.sub.3 /(YO.sub.2 + W'O + Z.sub.2 O.sub.5) 0.1 to 100 Solvent/ 1 to 1500 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) OH.sup.- /YO.sub.2 0 to 10 (M.sub.2/e O + R.sub.2/f O)/ 0.01 to 20 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) M.sub.2/e O/ 0 to 10 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) R.sub.2/f O/ 0.01 to 2.0 (YO.sub.2 + W'O + Z.sub.2 O.sub.5 + X.sub.2 O.sub.3) ______________________________________ wherein M is said alkali or alkaline earth metal cation, W' is said divalent element, X is said trivalent element, Y is said tetravalent element, Z is said pentavalent element, R comprises a mixture of component (a) an ion of the formula R 1 R 2 R 3 R 4 Q+, wherein Q is nitrogen or phosphorus and wherein at least one of R 1 , R 2 , R 3 and R 4 is aryl or alkyl of from 6 to about 36 carbon atoms or combinations thereof, the remainder of R 1 , R 2 , R 3 and R 4 being selected from the group consisting of hydrogen, alkyl of from 1 to 5 carbon atoms and combinations thereof, and component (b) an additional ion of the formula R 1 R 2 R 3 R 4 Q+ wherein R 1 , R 2 , R 3 and R 4 are selected from the group consisting of hydrogen, alkyl of 1 to 5 carbon atoms and combinations thereof, and wherein e and f are the weighted average valences of M and R, respectively.

Claim 42

The method of claim 33 wherein said reaction mixture has a composition, in terms of mole ratios within the following ranges: ______________________________________ Al.sub.2 O.sub.3 /SiO.sub.2 0 to 0.1 Solvent/SiO.sub.2 1 to 1500 OH.sup.- /SiO.sub.2 0 to 10 (M.sub.2/e O + R.sub.2/f O) 0.01 to 20 (SiO.sub.2 + Al.sub.2 O.sub.3) M.sub.2/e O/ 0 to 5 (SiO.sub.2 + Al.sub.2 O.sub.3) R.sub.2/f O/ 0.01 to 2 (SiO.sub.2 + Al.sub.2 O.sub.3) ______________________________________ wherein M is said alkali or alkaline earth metal cation, R is said organic directing agent, e and f are the weighted average valences of M and R, respectively.

Claim 43

In a method for synthesizing a composition of matter comprising an inorganic, non-layered, porous crystalline phase material having, after calcination, an arrangement of uniformly-sized pores having diameters of at least about 13 Angstrom Units, exhibiting an X-ray diffraction pattern with at least two peaks at positions greater than about 10 Angstrom Units d-spacing, at least one of which is at a position greater than about 18 Angstrom Units d-spacing, and no peaks at positions less than about 10 Angstrom Units d-spacing with relative intensity greater than about 20% of the strongest peak, which comprises (i) preparing a reaction mixture capable of forming said composition, said mixture comprising one or a combination of oxides selected from the group consisting of divalent element, trivalent element, tetravalent element and pentavalent element, organic directing agent and solvent or solvent mixture, said organic directing agent comprising an ion of the formula R 1 R 2 R 3 R 4 Q+, wherein Q is nitrogen or phosphorus and wherein at least one of R 1 , R 2 , R 3 and R 4 is aryl or alkyl of from 6 to about 36 carbon atoms or combinations thereof, the remainder of R 1 , R 2 , R 3 and R 4 being selected from the group consisting of hydrogen, alkyl of from 1 to 5 carbon atoms and combinations thereof, (ii) maintaining said mixture under sufficient conditions of pH, temperature and time for formation of said composition of matter and (iii) recovering said composition of matter, the improvement comprising contacting said recovered composition of matter of step (iii) with steam at elevated temperature.

Claim 44

In a method for synthesizing a composition of matter comprising an inorganic, non-layered, porous crystalline phase material having, after calcination, an arrangement of uniformly-sized pores having diameters of at least about 13 Angstrom Units, exhibiting an X-ray diffraction pattern with at least two peaks at positions greater than about 10 Angstrom Units d-spacing, at least one of which is at a position greater than about 18 Angstrom Units d-spacing, and no peaks at positions less than about 10 Angstrom Units d-spacing with relative intensity greater than about 20% of the strongest peak, which comprises (i) preparing a reaction mixture capable of forming said composition, said mixture comprising one or a combination of oxides selected from the group consisting of divalent element, trivalent element, tetravalent element and pentavalent element, organic directing agent and solvent or solvent mixture, said organic directing agent comprising an ion of the formula R 1 R 2 R 3 R 4 Q+, wherein Q is nitrogen or phosphorus and wherein at least one of R 1 , R 2 , R 3 and R 4 is aryl or alkyl of from 6 to about 36 carbon atoms or combinations thereof, the remainder of R 1 , R 2 , R 3 and R 4 being selected from the group consisting of hydrogen, alkyl of from 1 to 5 carbon atoms and combinations thereof, (ii) maintaining said mixture under sufficient conditions of pH, temperature and time for formation of said composition of matter and (iii) recovering said composition of matter, the improvement comprising contacting said recovered composition of matter of step (iii) with steam at elevated temperature.

Claim 45

The method of claim 42 wherein said crystalline phase has, after calcination, a hexagonal arrangement of uniformly-sized pores having diameters of at least about 13 Angstrom Units and exhibits a hexagonal electron diffraction pattern than can be indexed with a d 100 value greater than about 18 Angstrom Units.

Claim 46

The method of claim 42 wherein said crystalline phase has an X-ray diffraction pattern with at least one peak at a position greater than about 18 Angstrom Units d-spacing (4.909 degrees two-theta for Cu K-alpha radiation) with a relative intensity of 100 and exhibits an equilibrium benzene adsorption capacity of greater than about 15 grams benzene/100 grams crystal at 50 torr and 25° C.