Method to tailor zeolite silica-to-alumina ratio
The present disclosure is directed to a method of manufacture of zeolite. A sol-gel formulation includes a water-soluble fraction of ODSO as an additional component. The resulting products include zeolite with increased SAR relative to comparable sol-gel formulations without ODSO as a precursor. In addition, the SAR is increased by increasing the ODSO content during synthesis. In additional embodiments, zeolite yield is also increased.
1. A method for synthesis of zeolite comprising:
forming a homogeneous aqueous mixture of a silica source, an aluminum source, an alkali metal source, water and water-soluble oxidized disulfide oil (ODSO); and
heating the homogeneous aqueous mixture under conditions and for a time effective to form a crystalline zeolite as precipitate suspended in a supernatant, wherein the zeolite is characterized by a silica-to-alumina ratio that is greater than that of a comparative material, and wherein the comparative material is formed of approximately equivalent composition of components except for water instead of the added ODSO, and under approximately equivalent conditions and time.
2. The method of claim 1 , wherein an increase in a sub-ratio of water-soluble ODSO to water effects an increase in the silica-to-alumina ratio.
3. The method of claim 1 , wherein the zeolite is characterized by a zeolite yield, and wherein the zeolite yield is greater than that of the comparative material.
4. The method of claim 3 , wherein an increase in a sub-ratio of water-soluble ODSO to water effects an increase in the zeolite yield.
5. The method as in claim 1 , wherein the homogeneous aqueous mixture has a pH in the range of about 9-14, and wherein an increase in a sub-ratio of water-soluble ODSO to water effects a decrease in pH.
6. The method as in claim 1 , wherein the alkali metal source is sodium and the mass ratio of ODSO to sodium is in the range of about 0.1-10.
7. The method as in claim 1 , wherein the ODSO is derived from oxidation of disulfide oil compounds present in an effluent refinery hydrocarbon stream recovered following catalytic oxidation of mercaptans present in a mercaptan-containing hydrocarbon stream.
8. The method as in claim 1 , wherein the ODSO compounds have 3 or more oxygen atoms and include one or more compounds selected from the group consisting of (R′SOO—SO—R′), (R—SOO—SOO—R′), (R—SO—SOO—OH), (R—SOO—SOO—OH), (R—SOO—SO—OH), (R′—SO—SO—OR), (R′—SOO—SO—OR), (R′—SO—SOO—OR) and (R′—SOO—SOO—OR), wherein R and R′ can be the same or different C1-C10 alkyl or C6-C10 aryl.
9. The method as in claim 1 , wherein the ODSO compounds have 3 or more oxygen atoms and include two or more compounds selected from the group consisting of (R—SOO—SO—R′), (R—SOO—SOO—R′), (R—SO—SOO—OH), (R—SOO—SOO—OH), (R—SOO—SO—OH), (R′—SO—SO—OR), (R′—SOO—SO—OR), (R′—SO—SOO—OR) and (R′—SOO—SOO—OR), wherein R and R′ can be the same or different C1-C10 alkyl or C6-C10 aryl.
10. The method as in claim 1 , wherein the ODSO compounds have 3 or more oxygen atoms and include one or more compounds selected from the group consisting of (R—SOO—SO—R′), (R—SOO—SOO—R′), (R—SO—SOO—OH), (R—SOO—SOO—OH), (R—SO—SO—OH), (R—SOO—SO—OH), wherein R and R′ are C1-C10 alkyl or C6-C10 aryl.
11. The method as in claim 1 , wherein the aluminum source comprises aluminates, alumina, other zeolites, aluminum colloids, boehmites, pseudo-boehmites, aluminum hydroxides, aluminum salts, aluminum alkoxides, aluminum wire or alumina gels.
12. The method as in claim 1 , wherein the silica source comprises sodium silicate (water glass), rice husk, fumed silica, precipitated silica, colloidal silica, silica gels, zeolites, dealuminated zeolites, silicon hydroxides or silicon alkoxides.
13. The method as in claim 1 , wherein crystallization occurs in the absence of a seed.
14. The method as in claim 1 , wherein crystallization occurs in the presence of a seed.
15. The method as in claim 1 , wherein the homogeneous aqueous mixture further comprises a structure directing agent that is selected to influence the type of zeolite produced.
16. A method for synthesis of a first zeolite material and a second zeolite material comprising:
forming a first homogeneous aqueous mixture at a first ratio of a silica source, an aluminum source, an alkali metal source, water, an optional a structure directing agent, and water-soluble oxidized disulfide oil (ODSO);
heating the first homogeneous aqueous mixture under conditions and for a time effective to form a first crystalline zeolite as a first precipitate suspended in a supernatant, wherein the first zeolite material is characterized by a first silica-to-alumina ratio;
forming a second homogeneous aqueous mixture at a second ratio of a silica source, an aluminum source, an alkali metal source, water, an optional a structure directing agent, and water-soluble ODSO, wherein the second ratio is approximately the same as the first ratio except for a ratio of water and water-soluble ODSO in the solution, wherein an amount of ODSO in the second homogeneous aqueous mixture is greater than an amount of ODSO in the first homogeneous aqueous mixture;
heating the second homogeneous aqueous mixture approximately equivalent conditions and time as compared to the heating of the first homogeneous aqueous mixture to form a second crystalline zeolite as a second precipitate suspended in a supernatant, wherein the second zeolite material is characterized by a second silica-to-alumina ratio, and
wherein the second silica-to-alumina ratio is greater than the first silica-to-alumina ratio.
17. The method of claim 16 , wherein the first zeolite material and the second zeolite material zeolite are characterized by a first zeolite yield and a second zeolite yield, and wherein the second zeolite yield is greater than the first zeolite yield.