# US 11,999,617 B2 · Process for steam reforming of oxygenates and catalysts for use in the process

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- Number: US 11,999,617 B2
- Document ID: US11999617B2
- Status: Granted
- Kind: B2
- Application number: 17/967,139
- Filed: 2022-10-17
- Published: 2023-02-16
- Granted: 2024-06-04
- Earliest claimed: 2017-05-10
- Assignees: Haldor TopsøE A/S
- Applicants: Haldor TopsøE A/S
- Inventors: Poul Erik Højlund Nielsen; Brian Kjærgaard Olsen; Lived J. Lemus-Yegres
- Web page: https://patentgrep.com/patent/US11999617B2

## CPC

- C01B 3/326: characterised by the catalysts
- B01J 27/22: Carbides
- B01J 37/0201: {Impregnation}
- C01B 2203/0233: the reforming step being a steam reforming step
- C01B 2203/061: Methanol production
- C01B 2203/068: Ammonia synthesis
- C01B 2203/1058: Nickel catalysts
- C01B 2203/1076: Copper or zinc-based catalysts
- C01B 2203/1217: Alcohols
- C01B 2203/1229: Ethanol
- Y02P 20/52: using catalysts, e.g. selective catalysts
- 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
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

In a process for steam reforming of oxygenates, especially at low steam-to-carbon (S/C) ratios, a feed gas containing oxygenates, such as ethanol, is converted into syngas over a ternary carbide catalyst. Then the reformed gas is either transformed into desired chemicals or mixed into the feed stream to the reformer in a plant, such as an ammonia or methanol plant. The preferred ternary carbide is nickel zinc carbide.

## Claims

### Claim 1

A steam reforming catalyst, said steam reforming catalyst consisting of a nickel-containing catalyst for steam reforming, onto which a ternary carbide has been applied as a top layer, said ternary carbide being said nickel zinc carbide catalyst, and
in which said steam reforming catalyst is prepared by:
preparing a nickel-containing catalyst by a selected impregnation procedure, wherein the nickel-containing catalyst is reduced using hydrogen and methanol; and
feeding a reaction mixture into a stream of nitrogen and passing it over the catalyst at a suitable temperature under a pressure between ambient pressure and 5 MPa,
wherein said reaction mixture is obtained by:
mixing ethanol with water in a ratio corresponding to the reaction C2H5OH+3H2O <→2CO2+6H2; and
adding methanol,
wherein said temperature is from room temperature up to 800-900° C., and
wherein said steam reforming catalyst is configured for use in a process for steam reforming of oxygenates, in which a feed gas containing oxygenates is converted into syngas according to the reactions
C2H5OH+3H2O<→2CO2+6H2 or
C2H5OH+H2O<→CH4+CO2+H2
over a nickel zinc carbide catalyst, and which after use shows nickel solely in the form of alloys,
where the syngas is subsequently either transformed into desired chemicals or mixed into a feed stream to a reformer in a plant, wherein the plant is an ammonia or methanol plant,
wherein the impregnation procedure is an impregnation of a zinc-alumina spinel with nickel, wherein the Ni-load is 6 wt % Ni or less.

### Claim 2 (depends on 1)

The catalyst according to claim 1, wherein the impregnation procedure is selected from
co-impregnation of nickel and zinc onto alumina,
impregnation of a steam reforming nickel catalyst with zinc, and
impregnation of a zinc-alumina spinel with nickel.

### Claim 3 (depends on 1)

The catalyst according to claim 1, wherein adding methanol comprises adding 2100 ppmv methanol or less.