Crystalline silicoaluminophosphates
First Claim
1. Microporous crystalline silicoaluminophosphates the pores of which are uniform and have nominal diameters of greater than about 3 Angstroms and whose essential empirical chemical composition in the as-synthesized and anhydrous form is
wherein "R" represents at least one organic templating agent present in the intracrystalline pore system;
(Si.sub.x Al.sub.y P.sub.z)O.sub.2
"m" has a value of from 0.02 to 0.3;
"m" represents the moles of "R" present per mole of (Six Aly Pz)O2 ;
"x", "y" and "z" represent the mole fractions of silicon, aluminum and phosphorus respectively, present as tetrahedral oxides, said mole fractions being such that they are within the pentagonal compositional area defined by points ABCD and E of the ternary diagram which is FIG. 1 of the drawings.
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Abstract
A novel class of crystalline microporous silicoaluminophosphates is synthesized by hydrothermal crystallization of silicoaluminophosphate gels containing a molecular structure-forming templating agent. The class comprises a number of distinct species, each with a unique crystal structure. The compositions exhibit properties somewhat analogous to zeolitic molecular sieves which render them useful as adsorbent or catalysts in chemical reactions such as hydrocarbon conversions.
1196 Citations
38 Claims
- 1. Microporous crystalline silicoaluminophosphates the pores of which are uniform and have nominal diameters of greater than about 3 Angstroms and whose essential empirical chemical composition in the as-synthesized and anhydrous form is
- space="preserve" listing-type="equation">mR;
(Si.sub.x Al.sub.y P.sub.z)O.sub.2
wherein "R" represents at least one organic templating agent present in the intracrystalline pore system;
"m" has a value of from 0.02 to 0.3;
"m" represents the moles of "R" present per mole of (Six Aly Pz)O2 ;
"x", "y" and "z" represent the mole fractions of silicon, aluminum and phosphorus respectively, present as tetrahedral oxides, said mole fractions being such that they are within the pentagonal compositional area defined by points ABCD and E of the ternary diagram which is FIG. 1 of the drawings.- View Dependent Claims (2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 19, 30, 31, 32, 33, 34, 35, 36, 37, 38)
- 36. Process according to claim 35 wherein the organic templating agent is an amine.
- 37. Process according to claim 35 wherein the templating agent is selected from the group consisting of tetrapropylammonium ion;
- tetraethylammonium ion;
tripropylamine;
triethylamine;
triethanolamine;
piperidine;
cyclohexylamine;
2-methyl pyridine;
N,N-dimethylbenzylamine;
N,N-diethylethanolamine;
dicyclohexylamine;
N,N-dimethylethanolamine;
choline;
N,N-dimethylpiperazine;
1,4-diazabicyclo-(2,2,2)octane;
N-methyldiethanolamine;
N-methylethanolamine;
N-methylpiperidine;
3-methylpiperidine;
N-methylcyclohexylamine;
3-methylpyridine;
4-methylpyridine;
quinuclidine;
N,N'"'"'-dimethyl-1,4-diazabicyclo(2,2,2)octane ion;
tetramethylammonium ion;
tetrabutylammonium ion, tetrapentylammonium ion;
di-n-butylamine;
neopentylamine;
di-n-pentylamine;
isopropylamine;
t-butylamine;
ethylenediamine and 2-imidazolidone;
di-n-propylamine; and
a polymeric quaternary ammonium salt [(C14 H32 N2)]x+ wherein x is a value of at least 2.
- 38. Process for preparing a crystalline silicoaluminophosphate of claim 1 which comprises forming a reaction mixture having a composition expressed in terms of molar oxide rations of:
-
space="preserve" listing-type="equation">aR.sub.2 O;
bM.sub.2 O;
(Si.sub.x Al.sub.y P.sub.z)O.sub.2 ;
cH.sub.2 Owherein "R" is an organic templating agent;
"a" has a value great enough to constitute an effective concentration of "R" and is within the range >
0 to 3;
"M" is an alkali metal;
"b" has a value of zero to 2.5;
"c" has a value of from zero to 500;
"x", "y" and "z" represent the mole fractions, respectively, of silicon, aluminum and phosphorus in the (Six Aly Pz)O2 constituent, and each have a value of at least 0.01 and being within the quadrilateral compositional area defined by points f, g, h and i which is FIG. 3 of the drawings, the said points f, g, h and i representing the following values for "x", "y" and "z";
space="preserve" listing-type="tabular">______________________________________ Mole Fraction Point x y z ______________________________________ f 0.01 0.98 0.01 g 0.01 0.01 0.98 h 0.32 0.24 0.44 i 0.98 0.01 0.01;
______________________________________said reaction mixture having been formed by combining at least a portion of each of the aluminum and phosphorus sources in the substantial absence of the silicon source and thereafter combining the resulting mixture with the remaining constituents to form the complete reaction mixture, and thereafter crystallizing said complete reaction mixture at a temperature of from 100°
C. to about 250°
C. in a sealed reactor until crystals of the silicoaluminophosphate are formed.
- space="preserve" listing-type="equation">mR;
-
17. Silicoaluminophosphate material having a three-dimensional microporous framework structure of PO2+, AlO2- and SiO2 tetrahedral units, and whose essential empirical chemical composition on an anhydrous basis is:
-
space="preserve" listing-type="equation">mR;
(Si.sub.x Al.sub.y P.sub.z)O.sub.2wherein R represents at least one organic templating agent present in the intracrystalline pore system;
"m" represents the moles of "R" present per mole of (Six Aly Pz)O2 and has a value of from zero to 0.3;
"x", "y" and "z" represent respectively, the mole fractions of silicon, aluminum and phosphorus present in the oxide moiety, said mole fractions being within the compositional area bounded by points A, B, C, D and E on the ternary diagram which is FIG. 1, said silicoaluminophosphate having a characteristic X-ray powder diffraction pattern which contains at least the d-spacings set forth below in any one of Tables I, III, V, VII, IX, XIII, XVII, XXI, XXIII or XXV. - View Dependent Claims (18, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29)
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Specification