US4941963A — Synthesis of crystalline ZSM-11 structure

Claim 1

Independent Claim 223 words

A method for synthesizing a crystalline material exhibiting a characteristic X-ray diffraction pattern including values as shown in Table 1 TABLE 1 ______________________________________ Interplanar d-Spacing, (A) Relative Intensity (I/I.sub.o) ______________________________________ 11.2 ± .2 m 10.1 ± .2 m 6.73 ± .2 w 5.75 ± .1 w 5.61 ± .1 w 5.03 ± .1 w 4.62 ± .1 w 4.39 ± .08 w 3.86 ± .07 vs 3.86 ± .07 m 3.49 ± .07 w (3.07, 3.00 ± .05) w 2.01 ± .02 w ______________________________________ where vs=very strong (75-100), m=medium (25-49), and w=weak (0-24), which comprises (i) preparing a mixture capable of forming said material, said mixture comprising sources of alkali or alkaline earth metal (M), an oxide of trivalent element (X), an oxide of tetravalent element (Y), water and a directing agent (R), and having a composition, in terms of mole ratios, within the following ranges: ______________________________________ YO.sub.2 /X.sub.2 O.sub.3 at least 20 H.sub.2 O/YO.sub.2 5 to 200 OH.sup.- /YO.sub.2 0.01 to 2.0 M/YO.sub.2 0.01 to 3.0 R/YO.sub.2 0.02 to 2.0 ______________________________________ wherein R is a diquaternary ammonium of the formula: ##STR3## and wherein Bu is -butyl and n is 6 or 7; (ii) maintaining said mixture under sufficient conditions until crystals of said material are formed; and (iii) recovering said crystalline material from step (ii), said recovered crystalline material containing said R.

Claim 2

Independent Claim 223 words

A method for synthesizing a crystalline material exhibiting a characteristic X-ray diffraction pattern including values as shown in Table 1 TABLE 1 ______________________________________ Interplanar d-Spacing, (A) Relative Intensity (I/I.sub.o) ______________________________________ 11.2 ± .2 m 10.1 ± .2 m 6.73 ± .2 w 5.75 ± .1 w 5.61 ± .1 w 5.03 ± .1 w 4.62 ± .1 w 4.39 ± .08 w 3.86 ± .07 vs 3.86 ± .07 m 3.49 ± .07 w (3.07, 3.00 ± .05) w 2.01 ± .02 w ______________________________________ where vs=very strong (75-100), m=medium (25-49), and w=weak (0-24), which comprises (i) preparing a mixture capable of forming said material, said mixture comprising sources of alkali or alkaline earth metal (M), an oxide of trivalent element (X), an oxide of tetravalent element (Y), water and a directing agent (R), and having a composition, in terms of mole ratios, within the following ranges: ______________________________________ YO.sub.2 /X.sub.2 O.sub.3 at least 20 H.sub.2 O/YO.sub.2 5 to 200 OH.sup.- /YO.sub.2 0.01 to 2.0 M/YO.sub.2 0.01 to 3.0 R/YO.sub.2 0.02 to 2.0 ______________________________________ wherein R is a diquaternary ammonium of the formula: ##STR3## and wherein Bu is -butyl and n is 6 or 7; (ii) maintaining said mixture under sufficient conditions until crystals of said material are formed; and (iii) recovering said crystalline material from step (ii), said recovered crystalline material containing said R.

Claim 3

Dependent Claim 39 words

The method of claim 1 wherein said mixture has the following composition ranges: ______________________________________ YO.sub.2 /X.sub.2 O.sub.3 50 to 20,000 H.sub.2 O/YO.sub.2 10 to 100 OH.sup.- /YO.sub.2 0.1 to 0.5 M/YO.sub.2 0.1 to 1.0 R/YO.sub.2 0.05 to 0.5 ______________________________________

Claim 4

Dependent Claim 17 words

The method of claim 1 wherein said source of directing agent R is the hydroxide or halide.

Claim 5

Dependent Claim 17 words

The method of claim 2 wherein said source of directing agent R is the hydroxide or halide.

Claim 6

Dependent Claim 22 words

The method of claim 1 wherein said mixture further comprises seed crystals in sufficient amount to enhance synthesis of said crystalline material.

Claim 7

Dependent Claim 15 words

The method of claim 5 wherein said seed crystals have the structure of ZSM- 11.

Claim 8

Dependent Claim 29 words

The method of claim 1 wherein said X is aluminum, boron, iron, gallium, indium or a mixture thereof, and said Y is silicon, germanium, tin or a mixture thereof.

Claim 9

Dependent Claim 13 words

The method of claim 1 wherein X comprises aluminum and Y comprises silicon.

Claim 10

Dependent Claim 108 words

A mixture capable of forming crystals of ZSM-11 structure upon crystallization, said mixture comprising sources of alkali or alkaline earth metal (M), trivalent element (X) oxide selected from the group consisting of oxide of aluminum, boron, iron, gallium, indium and mixtures thereof; tetravalent element (Y) oxide selected from the group consisting of oxide of silicon, germanium, tin and mixtures thereof; water and diquaternary ammonium (R) of the formula: ##STR4## and having a composition, in terms of mole ratios, within the following ranges: ______________________________________ YO.sub.2 /X.sub.2 O.sub.3 at least 20 H.sub.2 O/YO.sub.2 5 to 200 OH.sup.- /YO.sub.2 0.01 to 2.0 M/YO.sub.2 0.01 to 3.0 R/YO.sub.2 0.02 to 2.0 ______________________________________

Claim 11

Dependent Claim 108 words

A mixture capable of forming crystals of ZSM-11 structure upon crystallization, said mixture comprising sources of alkali or alkaline earth metal (M), trivalent element (X) oxide selected from the group consisting of oxide of aluminum, boron, iron, gallium, indium and mixtures thereof; tetravalent element (Y) oxide selected from the group consisting of oxide of silicon, germanium, tin and mixtures thereof; water and diquaternary ammonium (R) of the formula: ##STR4## and having a composition, in terms of mole ratios, within the following ranges: ______________________________________ YO.sub.2 /X.sub.2 O.sub.3 at least 20 H.sub.2 O/YO.sub.2 5 to 200 OH.sup.- /YO.sub.2 0.01 to 2.0 M/YO.sub.2 0.01 to 3.0 R/YO.sub.2 0.02 to 2.0 ______________________________________

Claim 12

Dependent Claim 64 words

The method of claim 1 comprising replacing cations of the crystalline material recovered in step (iii), at least in part, by ion exchange with a cation or a mixture of cations selected from the group consisting of hydrogen and hydrogen precursors, rare earth metals and metals from Groups IIA, IIIA, IVA, IB, IIB, IIIB, IVB, VIB and VIII of the Periodic Table of Elements.

Claim 13

Dependent Claim 64 words

The method of claim 2 comprising replacing cations of the crystalline material recovered in step (iii), at least in part, by ion exchange with a cation or a mixture of cations selected from the group consisting of hydrogen and hydrogen precursors, rare earth metals and metals from Groups, IIA, IIIA, IVA, IB, IIB, IIIB, IVB, VIB and VIII of the Periodic Table of Elements.

Claim 14

Dependent Claim 15 words

The method of claim 10 wherein said replacing cation is hydrogen or a hydrogen precursor.

Claim 15

Dependent Claim 15 words

The method of claim 11 wherein said replacing cation is hydrogen or a hydrogen precursor.

Claim 16

Dependent Claim 7 words

The recovered crystalline material of claim 1.

Claim 17

Dependent Claim 7 words

The recovered crystalline material of claim 2.

Claim 18

Dependent Claim 10 words

The diquaternary ammonium R-containing product crystalline material of claim 10.

Claim 19

Dependent Claim 10 words

The diquaternary ammonium R-containing product crystalline material of claim 11.

Claim 20

Dependent Claim 10 words

The diquaternary ammonium R-containing product crystalline material of claim 12.

Claim 21

Dependent Claim 10 words

The diquaternary ammonium R-containing product crystalline material of claim 13.

Claim 22

Dependent Claim 35 words

A process for effecting catalytic conversion of an organic compound-containing feedstock which comprises contacting said feedstock under catalytic conversion conditions with a catalyst comprising an active form of the crystalline material product of claim 1.

Annuity Stage	Window Opens	Payment Deadline	Surcharge Period Until	Estimated Fee	Status
3.5 Years (Year 4)	1993-07-16	1994-01-15	1994-07-17	$2000.00	Window Closed / Lapsed
7.5 Years (Year 8)	1997-07-16	1998-01-15	1998-07-17	$3760.00	Window Closed / Lapsed
11.5 Years (Year 12)	2001-07-16	2002-01-15	2002-07-17	$7700.00	Window Closed / Lapsed

Synthesis of crystalline ZSM-11 structure

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