# US 10,865,116 B2 · Process for the synthesis of IZM-2 zeolite in the presence of a template, 1,6-bis(methylpiperidinium)hexane dihydroxide

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- Number: US 10,865,116 B2
- Document ID: US10865116B2
- Status: Granted
- Kind: B2
- Application number: 15/933,848
- Filed: 2018-03-23
- Published: 2018-09-27
- Granted: 2020-12-15
- Earliest claimed: 2017-03-24
- Assignees: Ifp Energies Nouvelles
- Applicants: IFP Energies Nouvelles
- Inventors: Raquel Martinez Franco; Nicolas Bats
- Web page: https://patentgrep.com/patent/US10865116B2

## CPC

- C01B 39/04: using at least one organic template directing agent, e.g. an ionic quaternary ammonium compound or an aminated compound
- B01J 29/70: of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- C01B 39/48: using at least one organic template directing agent
- C01B 7/19: Fluorine; Hydrogen fluoride
- C01D 1/02: Oxides
- C01F 11/02: Oxides or hydroxides (production of lime C04B2/00)
- C01P 2002/72: by d-values or two theta-values, e.g. as X-ray diagram
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- C01D: COMPOUNDS OF ALKALI METALS, i.e. LITHIUM, SODIUM, POTASSIUM, RUBIDIUM, CAESIUM, OR FRANCIUM (metal hydrides {monoborane, diborane or addition complexes thereof} C01B6/00; salts of oxyacids of halogens C01B11/00; peroxides, salts of peroxyacids C01B15/00; sulfides C01B17/22; thiosulfates, dithionites, polythionates C01B17/64; compounds containing selenium or tellurium C01B19/00; binary compounds of nitrogen with metals C01B21/06; azides C01B21/08; {compounds other than ammonia and cyanogen, containing nitrogen and other non-metals C01B21/082}; metal amides C01B21/092; nitrites C01B21/50; phosphides C01B21/50; {compounds of noble gases C01B23/0005}; phosphides C01B25/08; salts of oxyacids of phosphorus C01B25/16; carbides C01B32/90; compounds containing silicon C01B33/00; compounds containing boron C01B35/00; cyanides C01C3/08; salts of cyanic acid C01C3/14; salts of cyanamide C01C3/16; thiocyanates C01C3/20)
- C01F: COMPOUNDS OF THE METALS BERYLLIUM, MAGNESIUM, ALUMINIUM, CALCIUM, STRONTIUM, BARIUM, RADIUM, THORIUM, OR OF THE RARE-EARTH METALS (metal hydrides {monoborane, diborane or addition complexes thereof} C01B6/00; salts of oxyacids of halogens C01B11/00; peroxides, salts of peroxyacids C01B15/00; sulfides or polysulfides of magnesium, calcium, strontium, or barium C01B17/42; thiosulfates, dithionites, polythionates C01B17/64; compounds containing selenium or tellurium C01B19/00; binary compounds of nitrogen with metals C01B21/06; azides C01B21/08; {compounds other than ammonia or cyanogen containing nitrogen and non-metals and optionally metals C01B21/082; amides or imides of silicon C01B21/087}; metal {imides or} amides C01B21/092, {C01B21/0923}; nitrites C01B21/50; {compounds of noble gases C01B23/0005}; phosphides C01B25/08; salts of oxyacids of phosphorus C01B25/16; carbides C01B32/90; compounds containing silicon C01B33/00; compounds containing boron C01B35/00; compounds having molecular sieve properties but not having base-exchange properties C01B37/00; compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites, C01B39/00; cyanides C01C3/08; salts of cyanic acid C01C3/14; salts of cyanamide C01C3/16; thiocyanates C01C3/20; {double sulfates of magnesium with sodium or potassium C01D5/12; with other alkali metals C01D15/00, C01D17/00})
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS

## Abstract

A novel process is described for the preparation of a microporous crystalline solid, known as IZM-2 microporous solid or IZM-2 zeolite. This novel process consists of carrying out the synthesis of IZM-2 zeolite by conversion/transformation of a zeolite with structure type FAU in a fluorinated medium under hydrothermal conditions. In particular, said novel process consists of carrying out the synthesis of an IZM-2 zeolite in a fluorinated medium starting from a zeolite with structure type FAU used as the source of silicon and aluminium and a specific organic molecule or template comprising two quaternary ammonium functions, namely 1,6-bis(methylpiperidinium)hexane dihydroxide.

## Claims

### Claim 1

A process for preparing an IZM-2 zeolite, comprising at least the following steps:
i) mixing, in an aqueous medium,
at least one zeolite with structure type FAU having a molar ratio SiO2(fau)/Al2O3 (fau) of greater than or equal to 30,
at least one nitrogen-containing organic compound R, R being 1,6-bis(methylpiperidinium)hexane dihydroxide, and
at least one source of at least one fluoride anion,
optionally at least one additional source of an oxide XO2, wherein the molar ratio XO2/SiO2(fau) is in the range of 0 to 4,
the mixture having the following molar composition:
(XO2 + SiO2 (fau))/Al2O3 (fau)
in the range 30 to 600,
H2O/(XO2 + SiO2 (fau))
in the range 1 to 100,
R/(XO2 + SiO2 (fau))
in the range 0.01 to 0.6, and
BF/(XO2 + SiO2 (fau))
in the range 0.005 to 0.75,
in which
X is one or more tetravalent element(s) selected from the group consisting of the following elements: silicon, germanium, and titanium,
SiO2(fau) being the quantity of SiO2 supplied by the FAU zeolite,
Al2O3 (fau) being the quantity of Al2O3 supplied by the FAU zeolite, and
BF is a fluorine salt, in which B is a cation selected from the cations NH4+, Na+, K+ and Li+, or is hydrofluoric acid in an aqueous solution, and
ii) hydrothermal treatment of said mixture obtained from step i) at a temperature in the range of 120° C. to 200° C. for a period in the range of 1 day to 10 days, until said 1ZM-2 zeolite has been formed.

### Claim 2 (depends on 1)

The process as claimed in claim 1, in which said zeolite with structure type FAU is Y zeolite.

### Claim 3 (depends on 1)

The process as claimed in claim 1, in which the source BF of at least one anion is NH4F in aqueous solution.

### Claim 4 (depends on 1)

The process as claimed in claim 1, in which X is silicon.

### Claim 5 (depends on 1)

The process as claimed in claim 1, in which the additional source of an oxide XO2 is added in the mixing step i), wherein the molar ratio XO2/SiO2 (FAU) is in the range of 0 to 3.

### Claim 6 (depends on 1)

The process as claimed in claim 1, in which the reaction mixture obtained in step i) has the following molar composition:
(XO2 + SiO2 (FAU))/Al2O3 (FAU)
in the range 30 to 600,
H2O/(XO2 + SiO2 (FAU))
in the range 10 to 70,
R/(XO2 + SiO2 (FAU))
in the range 0.05 to 0.45, and
BF/(XO2 + SiO2 (FAU))
in the range 0.01 to 0.65.

### Claim 7 (depends on 1)

The process as claimed in claim 1, in which the reaction mixture obtained in step i) has the following molar composition:
(XO2 + SiO2 (FAU))/Al2O3 (FAU)
in the range 80 to 450,
H2O/(XO2 + SiO2 (FAU))
in the range 15 to 55
R/(XO2 + SiO2 (FAU))
in the range 0.085 to 0.4, and
BF/(XO2 + SiO2 (FAU))
in the range 0.02 to 0.55.

### Claim 8 (depends on 1)

The process as claimed in claim 1, in which the mixture of step i) also contains at least one source of at least one alkali metal and/or alkaline-earth metal M with valency n, wherein n is a whole number greater than or equal to 1, and M is lithium, potassium, sodium, magnesium or calcium or a mixture thereof.

### Claim 9 (depends on 1)

The process as claimed in claim 1, in which the hydrothermal treatment step ii) is carried out at a temperature in the range of 120° C. to 195° C.

### Claim 10 (depends on 1)

The process as claimed in claim 1, in which the hydrothermal treatment step ii) is carried out for a period in the range of 2 days to 11 days.

### Claim 11 (depends on 1)

The process as claimed in claim 1, in which the additional source of an oxide XO2 is added in the mixing step i).

### Claim 12 (depends on 1)

The process as claimed in claim 1, wherein X is silicon.

### Claim 13 (depends on 1)

The process as claimed in claim 1, wherein BF is a fluorine salt, in which B is a cation selected from the cations NH4+, Na+, K+ and Li+, in an aqueous solution.

### Claim 14 (depends on 1)

The process as claimed in claim 1, wherein BF is hydrofluoric acid in an aqueous solution.

### Claim 15 (depends on 1)

The process as claimed in claim 1, wherein the at least one zeolite with structure type FAU has a molar ratio SiO2(FAU)/Al2O3(FAU) of 30 to 100.

### Claim 16 (depends on 1)

The process as claimed in claim 1, wherein the at least one zeolite with structure type FAU has a molar ratio SiO2(FAU)/Al2O3(FAU) of 80.