Silicon substituted zeolite compositions and process for preparing same

Claim 2

Crystalline zeolite aluminosilicate having extraneous silicon atoms in its crystal lattice in the form of framework SiO 4 tetrahedra, and having in the dehydrated state a chemical composition expressed in terms of mole ratios of oxides 0.9±0.1M.sub.2/n O:Al.sub.2 O.sub.3 :xSiO.sub.2 wherein "M" is a cation having the valence of "n" and wherein said aluminosilicate has a combination of X-ray powder diffraction pattern and a value for "x" selected from the group consisting of: (i) a value for "x" of greater than 8 and an X-ray powder diffraction pattern having at least the d-spacings set forth in Table G or Table H or Table K or Table I; and (ii) a value for "x" of greater than 7, and an X-ray powder diffraction pattern having at least the d-spacings set forth in Table D; and (iii) a value for "x" of greater than 11, and an X-ray powder diffraction pattern having at least the d-spacings set forth in Table J; and (iv) a value for "x" of greater than 20, and an X-ray powder diffraction pattern having at least the d-spacings set forth in Table L.

Claim 3

A crystalline aluminosilicate having at least some of its original framework aluminum atoms replaced by extraneous silicon atoms and having the chemical composition [Al.sub.(a-N) Si.sub.b+(N-Δz) □.sub.z ]O.sub.2 wherein Al.sub.(a-N) represents the mole fraction of aluminum tetrahedra in the product zeolite; "a" represents the mole fraction of aluminum tetrahedra in the original zeolite; "N" represents the mole fraction of aluminum tetrahedra removed from the original zeolite, and has a value of at least 0.3a; Si b+ (N-Δz) represents the mole fraction of silicon tetrahedra in the product zeolite; "b" represents the mole fraction of silicon tetrahedra in the original zeolite; (N-Δz) represents the mole fraction of silicon tetrahedra resulting from the substitution of extraneous silicon into the crystal lattice; "□" represents the framework defect sites; "z" represents the mole fraction of framework defect sites; Δ"z" represents the difference between the mole fraction of framework defect sites of the original zeolite and the zeolite containing the extraneous silicon atoms and has a value of less than 0.08; (N-Δz)/N has a value at least as great as 0.5, and possesses a combination of X-ray powder diffraction patterns and a value for the term [b+(N-Δz)]/(a-N) selected from the group of such combinations consisting of (i) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table J and a value for [b+(N-Δz)]/(a-N) of at least 5.5; and (ii) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table L and a value for [b+(N-Δz)]/(a-N) of at least greater than 10; and (iii) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table D and a value for [b+(N-Δz)]/(a-N) of at least 4.0; and (iv) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table G and a value for [b+(N-Δz)]/(a-N) of at least 4.0; and (v) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table H and a value for [b+(N-Δz)]/(a-N) of at least 4.0; and (vi) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table I and a value for [b+(N-Δz)]/(a-N) of at least 4.0; and (vii) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table K and a value for [b+(N-Δz)]/(a-N) of at least 4.0.

Claim 4

A crystalline aluminosilicate having at least some of its original framework aluminum atoms replaced by extraneous silicon atoms and having the chemical composition [Al.sub.(a-N) Si.sub.b+(N-Δz) □.sub.z ]O.sub.2 wherein Al.sub.(a-N) represents the mole fraction of aluminum tetrahedra in the product zeolite; "a" represents the mole fraction of aluminum tetrahedra in the original zeolite; "N" represents the mole fraction of aluminum tetrahedra removed from the original zeolite, and has a value of at least 0.3a; Si b+ (N-Δz) represents the mole fraction of silicon tetrahedra in the product zeolite; "b" represents the mole fraction of silicon tetrahedra in the original zeolite; (N-Δz) represents the mole fraction of silicon tetrahedra resulting from the substitution of extraneous silicon into the crystal lattice; "□" represents the framework defect sites; "z" represents the mole fraction of framework defect sites; Δ"z" represents the difference between the mole fraction of framework defect sites of the original zeolite and the zeolite containing the extraneous silicon atoms and has a value of less than 0.08; (N-Δz)/N has a value at least as great as 0.5, and possesses a combination of X-ray powder diffraction patterns and a value for the term [b+(N-Δz)]/(a-N) selected from the group of such combinations consisting of (i) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table J and a value for [b+(N-Δz)]/(a-N) of at least 5.5; and (ii) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table L and a value for [b+(N-Δz)]/(a-N) of at least greater than 10; and (iii) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table D and a value for [b+(N-Δz)]/(a-N) of at least 4.0; and (iv) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table G and a value for [b+(N-Δz)]/(a-N) of at least 4.0; and (v) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table H and a value for [b+(N-Δz)]/(a-N) of at least 4.0; and (vi) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table I and a value for [b+(N-Δz)]/(a-N) of at least 4.0; and (vii) an X-ray powder diffraction pattern having at least the d-spacings set forth in Table K and a value for [b+(N-Δz)]/(a-N) of at least 4.0.

Claim 5

Crystalline aluminosilicate according to claim 2 wherein the value of Δz is less than 0.05.

Claim 6

Crystalline aluminosilicate composition according to claim 1 wherein "x" has a value of from 8 to 120, the extraneous silicon atoms are present in an amount of at least 1.0 per 10,000 A 3 , and the aluminosilicate has an X-ray powder diffraction pattern having at least the d-spacings set forth in Table D.

Claim 7

Crystalline aluminosilicate composition according to claim 1 wherein "x" has a value of from 8 to 60, the extraneous silicon atoms are present in an amount of at least 1.0 per 10,000 A 3 , and the aluminosilicate has an X-ray powder diffraction pattern having at least the d-spacings set forth in Table G.

Claim 8

Crystalline aluminosilicate composition according to claim 1 wherein "x" has a value of from 8 to 20, the extraneous silicon atoms are present in an amount of at least 1.0 per 10,000 A 3 , and the aluminosilicate has an X-ray powder diffraction pattern having at least the d-spacings set forth in Table I.

Claim 9

Crystalline aluminosilicate composition according to claim 1 wherein the extraneous silicon atoms are present in an amount of at least 1.0 per 10,000 A 3 , and the aluminosilicate has an X-ray powder diffraction pattern having at least the d-spacings set forth in Table H.

Claim 10

Crystalline aluminosilicate composition according to claim 1 wherein "x" has a value of from 12 to 20, the extraneous silicon atoms are present in an amount of at least 1.0 per 10,000 A 3 , and the aluminosilicate has an X-ray powder diffraction pattern having at least the d-spacings set forth in Table J.

Claim 11

Crystalline aluminosilicate composition according to claim 1 wherein "x" has a value of from 8 to 20, the extraneous silicon atoms are present in an amount of at least 1.0 per 10,000 A 3 , and the aluminosilicate has an X-ray powder diffraction pattern having at least the d-spacings set forth in Table K.

Claim 12

Crystalline aluminosilicate composition according to claim 1 wherein "x" has a value of from 22 to 60, the extraneous silicon atoms are present in an amount of at least 1.0 per 10,000 A 3 , and the aluminosilicate has an X-ray powder diffraction pattern having at least the d-spacings set forth in Table L.