# US 2014/0194542 A1 · Catalytic process for the conversion of a synthesis gas to hydrocarbons

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- Number: US 2014/0194542 A1
- Document ID: US20140194542A1
- Status: Published application
- Kind: A1
- Application number: 14/123,235
- Filed: 2012-05-31
- Published: 2014-07-10
- Earliest claimed: 2011-06-01
- Assignees: Sicat GmbH & Co. KG; Total SA; Centre National De La Recherche Scientifique; Universite De Strasbourg
- Inventors: Francis Luck; Charlotte Pham; Patrick Nguyen; Cuong Pham-Huu; Benoit De Tymowski
- Web page: https://patentgrep.com/patent/US20140194542A1

## CPC

- C07C 1/044: {containing iron}
- B01J 21/06: Silicon, titanium, zirconium or hafnium; Oxides or hydroxides thereof
- B01J 23/745: Iron
- B01J 23/75: Cobalt
- B01J 23/78: with alkali- or alkaline earth metals
- B01J 23/83: with rare earths or actinides
- B01J 23/8906: {Iron and noble metals}
- B01J 23/8913: {Cobalt and noble metals}
- B01J 27/22: Carbides
- B01J 27/224: Silicon carbide
- B01J 35/612: {less than 10 m2/g}
- B01J 35/633: {less than 0.5 ml/g}
- B01J 35/647: {2-50 nm}
- B01J 35/651: {50-500 nm}
- B01J 37/0009: {Use of binding agents; Moulding; Pressing; Powdering; Granulating; Addition of materials ameliorating the mechanical properties of the product catalyst}
- B01J 37/0201: {Impregnation}
- C07C 1/0435: {containing a metal of group 8 or a compound thereof}
- C10G 2/332: {of the iron-group}
- B01J 35/34: Mechanical properties
- B01J 2235/30: Scanning electron microscopy; Transmission electron microscopy
- C10G 2300/1022: Fischer-Tropsch products
- C10G 2300/703: Activation
- C07C: ACYCLIC OR CARBOCYCLIC COMPOUNDS
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- C10G: CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION (cracking to hydrogen or synthesis gas C01B; cracking or pyrolysis of hydrocarbon gases to individual hydrocarbons or mixtures thereof of definite or specified constitution C07C; cracking to cokes C10B); RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES

## Abstract

Catalytic process for the partial conversion of a gaseous mixture containing carbon monoxide and hydrogen into a mixture of hydrocarbons, including bringing the said gaseous mixture into contact with a solid catalyst, the solid catalyst having a porous support with a composite material including SiC and a titanium carbide and/or a titanium oxide, and an active phase. The support is prepared in the form of grains, beads, or extrudates, or in the form of cylinders or sheets of cellular foam.

## Claims

### Claim 1

Process of at least partial catalytic conversion of a gaseous mixture containing CO and H2 in a mixture of hydrocarbons, comprising a step of placing said gaseous mixture in contact with a solid catalyst, said solid catalyst comprising:
a porous support comprising a composite material comprising SiC and a titanium carbide (composite called “SiC/TiC”) and/or a titanium oxide (composite called “SiC/TiO2”), and
an active phase.

### Claim 2 (depends on 1)

Process according to claim 1, wherein said composite material has been prepared by a method including the preparation of a mixture comprising at least one silicon source, at least one carbon source and at least one titanium source and optionally binders and forming agents, this preparation being followed by at least one heat treatment that is intended to transform said silicon source at least partially into silicon carbide and at least part of said titanium source into titanium carbide, said heat treatment preferably being at least partially performed at a temperature of between 1200° C. and 1450° C.

### Claim 3 (depends on 2)

Process according to claim 2, wherein said method for preparing said composite material also includes a step of additional oxidation at a temperature of at least 350° C., and preferably at least 400° C., in order to partially or totally transform the titanium carbide into titanium dioxide.

### Claim 4 (depends on 1)

Process according to claim 1, wherein the content of active phase with respect to the total mass of said porous support with its active phase is between 1 and 50% by mass, preferably between 5% and 35% and even more preferably between 5% and 30%.

### Claim 5 (depends on 1)

Process according to claim 1, wherein said active phase includes primarily cobalt and iron, and optionally the other of the two metals, and optionally one or more transition metals from groups 7, 8, 9 and/or 10.

### Claim 6 (depends on 1)

Process according to claim 1, wherein said active phase includes a promoter, preferably with in a content not exceeding 2% by mass.

### Claim 7 (depends on 6)

Process according to claim 6, characterized in that said promoter is selected from the group formed by: ruthenium (preferred promoter), platinum, rhenium, rhodium, iridium, palladium, rare earth elements and oxides thereof, alkaline earth elements and oxides thereof, and transition metals and oxides thereof.

### Claim 8 (depends on 1)

Process according to claim 1, wherein said porous support has a specific BET surface area greater than 5 m2/g, preferably greater than 30 m2/g, more preferably greater than 40 m2/g, and even more preferably greater than 60 m2/g.

### Claim 9 (depends on 1)

Process according to claim 1, wherein said porous support has a molar content of titanium with respect to the molar sum of Si+Ti of between 0.5% and 15%, and preferably between 0.5% and 10%.

### Claim 10 (depends on 1)

Process according to claim 1, wherein said porous support has a microporous surface area greater than 10 m2/g, and preferably greater than 20 m2/g.

### Claim 11 (depends on 10)

Process according to claim 10, characterized in that said porous support has a porous volume in the range of 30 nm and 300 nm measured by mercury intrusion greater than 0.12 cm3/g, preferably greater than 0.15 cm3/g and even more preferably greater than 0.20 cm3/g.

### Claim 12 (depends on 1)

Process according to claim 1, characterized in that said support is in the form of pellets, beads, extrudates or in the form of a cellular foam.

### Claim 13 (depends on 1)

Process for preparing and activating a catalyst for use in the catalytic conversion process according to claim 1, said preparation and activation process including:
(a) at least one step of depositing active phase precursor on a porous support comprising a composite material of the SiC/TiC and/or SiC/TiO2 type;
(b) at least one phase of activating said active phase precursor in order to form the active phase.

### Claim 14 (depends on 13)

Process according to claim 13, characterized in that said precursor deposition phase includes at least one phase of impregnating said support with a solution of an active phase precursor, followed by a step of drying and a step of calcination.

### Claim 15 (depends on 14)

Process according to claim 14, characterized in that said calcination is performed at a temperature of between 250° C. and 450° C. for 1 to 14 hours, preferably between 300° C. and 400° C. for 4 to 16 hours.