IP Library › Granted Patent US 12,600,736
Granted Patent B2
US 12,600,736 · App. 17/857,671 · Granted Apr 14, 2026

Methods for synthesis of hierarchically ordered crystalline microporous materials with long-range mesoporous order

Inventors: Rajesh Kumar Parsapur (Thuwal, SA); Robert P. Hodgkins (Dhahran, SA); Omer Refa Koseoglu (Dhahran, SA); Kuo-Wei Huang (Thuwal, SA); Anissa Bendjeriou Sedjerari (Thuwal, SA)
Assignees: Saudi Arabian Oil Company; King Abdullah University of Science and Technology
C07F7/1892C01B33/2853C01P2002/72C01P2002/77C01P2004/04
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Quick Facts
Patent No.
US 12,600,736
App. No.
17/857,671
Granted
Apr 14, 2026
Kind
B2
Abstract

Methods for synthesis of hierarchically ordered zeolites and zeolite-type materials are provided. Synthesized hierarchically ordered zeolites and zeolite-type materials formed according to the methods herein possess a high-degree of well-defined long-range mesoporous ordering. The methods include base-mediated reassembly, by dissolution of the parent material to the level of oligomeric structural building units of the parent material, and minimizing or avoiding amorphization/structural collapse. The dissolution and self-assembly is comprehensively controlled to produce hierarchically ordered zeolites and zeolite-type materials according to the methods herein.

Claims (22)

1 . A method for synthesis of hierarchically ordered zeolite having FAU framework having long-range mesoporous ordering by dissolution/incision of a parent zeolite having FAU framework having micropores of 7.4 angstroms into oligomeric components, and reorganization into hierarchically ordered mesostructures, the method comprising:

mixing the parent zeolite having FAU framework,

a base selected from the group consisting of ammonia, ammonium hydroxide and urea, and

a supramolecular template that is a quaternary ammonium moiety comprising a terminal C 6 -C 24 alkyl group and a head group comprising a moiety selected from the group consisting of organosilanes, hydroxysilyls, and alkoxysilyls;

to form an aqueous suspension,

hydrothermally treating the aqueous suspension at a temperature of 110-250° C. to dissolve the parent zeolite having FAU framework by forming oligomeric units of the parent zeolite having FAU framework, and then form a solid hierarchically ordered mesostructure comprising mesopore periodicity repeating over a length of greater than 50 nm.

2 . The method as in claim 1 , wherein the aqueous suspension further comprises an ionic co-solute that is separate from an anion associated with the supramolecular template.

3 . The method as in claim 2 , wherein the ionic co-solute is selected from the group consisting of CO 3 2− , SO 4 2− , S2O 3 2− , H 2 PO 4 − , F − , Cl − , Br − , NO 3 − , I − , ClO 4 − , SCN − and C 6 H 5 O 8 −3 .

4 . The method as in claim 2 , wherein the ionic co-solute is selected from the group consisting of SO 4 2− , NO 3 − , and ClO 4 − .

5 . The method as in claim 2 , wherein the ionic co-solute comprises NO 3 − .

6 . The method as in claim 2 , wherein the ionic co-solute comprises SO 4 2− .

7 . The method as in claim 2 , wherein the ionic co-solute comprises ClO 4 − .

8 . The method as in claim 1 , wherein the supramolecular template contains two quaternary ammonium groups, wherein an alkyl group bridging the quaternary ammonium groups contains 1-10 carbon atoms.

9 . The method as in claim 1 , wherein the supramolecular template is dimethyloctadecyl(3-trimethoxysilyl-propyl)-ammonium as a cation paired with an anion selected from the group consisting of Cl − , Br − , OH − , F − and I − .

10 . The method as in claim 1 , wherein the base is provided at a concentration in the aqueous suspension of 0.1-5 wt %.

11 . The method as in claim 1 , wherein the base is urea.

12 . The method as in claim 1 , wherein the as-formed hierarchically ordered mesostructures are calcined.

13 . The method as in claim 1 , wherein hydrothermally treating occurs at 110-180° C.

14 . The method as in claim 9 , wherein hydrothermally treating occurs at 110-150° C. for 24-96 hours.

15 . The method as in claim 1 , wherein the zeolite having FAU framework comprises zeolite H-Y.

16 . The method as in claim 1 , wherein the supramolecular template is [2,3-bis(dodecanoyloxy)-propyl](3-(trimethoxysilyl)propyl)-dimethylammonium as a cation paired with an anion selected from the group consisting of Cl − , Br − , OH − , F − and I − .

17 . The method as in claim 1 , wherein the supramolecular template is dimethylhexadecyl[3-(trimethoxysilyl)propyl]ammonium as a cation paired with an anion selected from the group consisting of Cl − , Br − , OH − , F − and I − .

Assignments (2)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jul 5, 2022
From: HODGKINS, ROBERT P.; KOSEOGLU, OMER REFA
To: SAUDI ARABIAN OIL COMPANY
Reel/Frame 060401/0110 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jul 5, 2022
From: PARSAPUR, RAJESH KUMAR; HUANG, KUO-WEI; SEDJERARI, ANISSA BENDJERIOU
To: KING ABDULLAH UNIVERSITY OF SCIENCE AND TECHNOLOGY
Reel/Frame 060401/0310 →
Continuity (1)
Related Publication 20240010662A1 · Jan 11, 2024
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