Continuous synthesis of a titanosilicate zeolitic material, said zeolitic material, molding prepared thereof, and their use

Patent metadata

Field	Value
Publication number	US-12478959-B2
Application number	US-202017785856-A
Country	US
Kind code	B2
Filing date	Dec 18, 2020
Priority date	Dec 19, 2019
Publication date	Nov 25, 2025
Grant date	Nov 25, 2025

Abstract

The present invention relates to a specific continuous process for preparing a zeolitic material having a framework structure type selected from the group consisting of MFI, MEL, IMF, SVY, FER, SVR, and intergrowth structures of two or more thereof, preferably an MFI- and/or MEL-type framework structure, comprising Si, Ti, and O, and to a zeolitic material as obtainable and/or obtained according to said process. Further, the present invention relates to a process for preparing a molding, and to a molding obtainable and/or obtained according to said process. Yet further, the present invention relates to a use of said zeolitic material and molding.

First claim

The invention claimed is:

1 . A continuous process for preparing a zeolitic material having an MFI framework structure type comprising TS-1, comprising Si, Ti, and O, said process comprising
(i) preparing a mixture comprising one or more sources of Si, one or more sources of Ti, one or more tetraalkylammonium cation R 1 R 2 R 3 R 4 N + -containing compounds as structure directing agent, and water; (ii) continuously feeding the mixture prepared in (i) into a continuous flow reactor; and (iii) crystallizing the zeolitic material having an MFI framework structure type, wherein the mixture is heated to a temperature in the range of from 130 to 220° C., wherein R 1 , R 2 , R 3 , and R 4 independently from one another stand for alkyl, and wherein the H 2 O:Si molar ratio of water to the one or more sources of Si calculated as SiO 2 in the mixture prepared in (i) is in the range of from 3 to 11; wherein the mixture constituting the feed crystallized in (iii) consists of a first liquid phase and a second liquid phase, wherein the first liquid phase is an aqueous phase comprising water, and the second liquid phase comprises a lubricating agent; wherein the lubricating agent comprises one or more fluorinated compounds or a liquid paraffin.

2 . The process of claim 1 , wherein the H 2 O: Si molar ratio of water to the one or more sources of Si calculated as SiO 2 in the mixture prepared in (i) is in the range of from 4 to 10.

3 . The process of claim 1 , wherein the continuous flow reactor is selected among a tubular reactor, a ring reactor, and a continuously oscillating reactor.

4 . The process of claim 1 , wherein the mixture prepared in (i) and crystallized in (iii) displays a molar ratio of the one or more tetraalkylammonium cation R 1 R 2 R 3 R 4 N + -containing compounds to the one or more sources of Si calculated as Si in the range of from 0.001 to 1.5.

5 . The process of claim 1 , wherein the Si: Ti molar ratio of the mixture prepared in (i) is in the range of from 1 to 500.

6 . The process of claim 1 , wherein in (iii) the mixture is heated under autogenous pressure.

7 . The process of claim 1 , wherein the mixture prepared in (i) is directly fed to the continuous flow reactor in (ii), wherein while being fed to the continuous flow reactor in (ii), the mixture prepared in (i) is pre-heated.

8 . The process of claim 1 , wherein the process further comprises
(iv) treating the reaction product effluent continuously exiting the reactor in (iii) with a liquid comprising one or more solvents and/or via expansion of the reaction product effluent; and/or (v) isolating the zeolitic material obtained in (iii) or (iv); (vi) optionally washing the zeolitic material obtained in (iii), (iv) or (v); (vii) drying the zeolitic material obtained in (iii), (iv), (v), or (vi); and/or (viii) calcining the zeolitic material obtained in (iii), (iv), (v), (vi), or (vii).

9 . The process of claim 1 , wherein the H 2 O:Si molar ratio of water to the one or more sources of Si calculated as SiO 2 in the mixture prepared in (i) is in the range of from 5 to 9.

10 . The process of claim 1 , further comprising:
(B) mixing the prepared zeolitic material having a framework structure type MFI, comprising Si, Ti, and O—with one or more binders; (C) optionally kneading of the mixture obtained in step (B); (D) molding of the mixture obtained in step (B) or (C) to obtain one or more moldings; (E) drying of the one or more moldings obtained in step (D); and (F) calcining of the dried molding obtained in step (E).

11 . The process of claim 10 , further comprising:
(G) subjecting the calcined molding obtained in step (F) to a hydrothermal treatment.

12 . The process of claim 1 , wherein the continuous feeding in (ii) is performed at a liquid hourly space velocity in the range of from 0.05 to 5 h−1;
wherein the volume of the continuous flow reactor is in the range of from 50 cm3 to 75 m3; and
wherein the surface of the inner wall of the continuous flow reactor is lined with an organic polymer material.

Assignees

• Basf Se

Inventors

• Schreyer Hannah
• Parvulescu Andrei-Nicolae
• Mueller Ulrich
• Riedel Dominic
• Mormul Jaroslaw Michael
• Boehling Ralf

Classifications

• B01J2235/05

  Nuclear magnetic resonance [NMR] · CPC title

• B01J2235/15

  X-ray diffraction · CPC title

• B01J37/10

  in the presence of water, e.g. steam · CPC title

• B01J37/06

  Washing {(B01J37/0009, B01J37/0018 take precedence)} · CPC title

• B01J37/04

  Mixing {(B01J37/0009, B01J37/0018 take precedence)} · CPC title