Control of morphology of mesoporous aluminosilicate or pure-silica molecular sieves by effect of alcohol

A method for preparing a molecular sieve having a hollow spherical morphology with a pillar inside comprising:

• a) preparing an aqueous mixture having a molar ratio composition of (a) R1R2R3R4Q+X−:(b) SiO2:(c) M(OH)n:(d) alcohol:(e) H2O, wherein a=1, 0.3≦b≦3.0, 0.24≦c≦2.78, 0.1≦d≦3.0 and 50≦e≦2000,
• wherein at least one of R1, R2, R3 and R4 is an alkyl chain with 6 to 20 carbon atoms and the remainder of R1, R2, R3 and R4 are alkyl chains with 1 to 6 carbon atoms,
• wherein Q is selected from the group consisting of nitrogen atom and phosphorous atom,
• wherein X− is a counterion,
• wherein M is an alkali metal when n=1,
• wherein M is an alkaline earth metal when n=2;
• b) stirring the aqueous mixture at a temperature of about 0° C. to about room temperature for about 10 to about 30 minutes to form a gel mixture;
• c) slowly adding an acid to the gel mixture in an amount determined by H+/surfactant molar ratio=0.2 to 2 within a period of about 10 to about 60 minutes, the stirring being maintained in the period and a final pH value of about 10 being reached;
• d) heating the resulting mixture of step c) at a temperature of about 20 to about 250° C. for about 1 to about 480 hours to form the molecular sieve;
• e) recovering the molecular sieve by filtration and washing the molecular sieve with deionized water;
• and
• f) calcining the molecular sieve to remove the R1R2R3R4Q+ in the pores of the molecular sieve at a temperature of about 500 to about 900° C. for about 6 to about 12 hours with a heating rate of about 0.5 to about 2° C./min.

A method for preparing a molecular sieve of hollow spherical morphology comprising:

• a) preparing an aqueous mixture having a molar ratio composition of (a) R1R2R3R4Q30 X−:(b) SiO2:(c) Al2O3:(d) M(OH)n:(e) alcohol:(f) H2O, wherein a=1, 0.3≦b≦3.0, 0<c≦0.3, 0.24≦d≦2.78, 0.1≦e≦3.0 and 50≦f≦2000,
• wherein at least one of R1, R2, R3 and R4 is an alkyl chain with 6 to 20 carbon atoms and the remainder of R1, R2, R3 and R4 are alkyl chains with 1 to 6 carbon atoms,
• wherein Q is selected from the group consisting of nitrogen atom and phosphorous atom,
• wherein X− is a counterion,
• wherein M is an alkali metal when n=1,
• wherein M is an alkaline earth metal for n=2;
• b) stirring the aqueous mixture at a temperature of about 0° C. to about room temperature for about 10 to about 30 minutes to form a gel mixture;
• c) slowly adding an acid to the gel mixture in an amount determined by H+/surfactant molar ratio=0.2 to 2 within a period of about 10 to about 60 minutes, the stirring being maintained in the period and a final pH value of about 10 being reached;
• d) heating the resulting mixture of step c) at a temperature of about 20 to about 250° C. for about 1 to about 480 hours to form the molecular sieve;
• e) recovering the molecular sieve by filtration and washing the molecular sieve with deionized water;
• and
• f) calcining the molecular sieve to remove the R1R2R3R4Q+ in the pores of the molecular sieve at a temperature of about 500 to about 900° C. for about 6 to about 12 hours with a heating rate of about 0.5 to about 2° C./min.

A method for preparing a molecular sieve of solid spherical morphology comprising:

• a) preparing an aqueous mixture having a molar ratio composition of (a) R1R2R3R4Q+X−:(b) SiO2:(c) tetraethylorthosilicate:(d) M(OH)n:(e) alcohol:(f) H2O, wherein a=1, 0.3≦b≦3.0, 0<c≦10, 0.24≦d≦2.78, 0.1≦e≦3.0 and 50≦f≦2000,
• wherein at least one of R1, R2, R3 and R4 is an alkyl chain with 6 to 20 carbon atoms and the remainder of R1, R2, R3 and R4 are alkyl chains with 1 to 6 carbon atoms,
• wherein Q is selected from the group consisting of nitrogen atom and phosphorous atom,
• wherein X− is a counterion,
• wherein M is an alkali metal for n=1,
• wherein M is an alkaline earth metal for n=2;
• b) stirring the aqueous mixture at a temperature of about 0° C. to about room temperature for about 10 to about 30 minutes to form a gel mixture;
• c) slowly adding an acid to the gel mixture in an amount determined by H+/surfactant molar ratio=0.2 to 2 within a period of about 10 to about 60 minutes, the stirring being maintained in the period and a final pH value of about 10 being reached;
• d) heating the resulting mixture of step c) at a temperature of about 20 to about 250° C. for about 1 to about 480 hours to form the molecular sieve;
• e) recovering the molecular sieve by filtration and washing the molecular sieve with deionized water;
• and
• f) calcining the molecular sieve to remove the R1R2R3R4Q+ in the pores of the molecular sieve at a temperature of about 500 to about 900° C. for about 6 to about 12 hours with a heating rate of about 0.5 to about 2° C./min.