# US 12,005,427 B2 · Catalyst for methanation reaction and method for preparing methane

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- Number: US 12,005,427 B2
- Document ID: US12005427B2
- Status: Granted
- Kind: B2
- Application number: 17/946,747
- Filed: 2022-09-16
- Published: 2023-05-11
- Granted: 2024-06-11
- Earliest claimed: 2021-11-10
- Assignees: Industrial Technology Research Institute
- Applicants: Industrial Technology Research Institute
- Inventors: Yen-Chih Chen; Man-Yin Lo; Hsi-Yen Hsu; Ying-Chieh Lee; Yuan-Peng Du
- Web page: https://patentgrep.com/patent/US12005427B2

## CPC

- B01J 23/755: Nickel
- B01J 35/397: {Egg shell like}
- B01J 21/066: {Zirconium or hafnium; Oxides or hydroxides thereof}
- B01J 23/10: of rare earths
- B01J 23/83: with rare earths or actinides
- B01J 35/393: {Metal or metal oxide crystallite size}
- B01J 35/45: Nanoparticles
- B01J 35/51: Spheres
- C07C 1/043: {characterised by the composition}
- B01J 2235/30: Scanning electron microscopy; Transmission electron microscopy
- C07C 2521/06: Silicon, titanium, zirconium or hafnium; Oxides or hydroxides thereof
- C07C 2523/10: of rare earths
- C07C 2523/755: Nickel
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- C07C: ACYCLIC OR CARBOCYCLIC COMPOUNDS

## Abstract

A catalyst for methanation reaction and a method for preparing methane are provided. The catalyst for methanation reaction includes a core, a shell encapsulating the core, and an active metal. The core includes cerium dioxide (CeO2), the shell includes zirconium dioxide (ZrO2), and the active metal is in particle form and is disposed on an outer surface of the shell layer.

## Claims

### Claim 1

A catalyst for methanation reaction, comprising:
a core, wherein the core comprises cerium dioxide (CeO2);
a shell encapsulating the core, wherein the shell comprises zirconium dioxide (ZrO2); and
an active metal, wherein the active metal is in particle form and is disposed on an outer surface of the shell.

### Claim 2 (depends on 1)

The catalyst for methanation reaction as claimed in claim 1, wherein a weight ratio of the core to the shell is 2:1 to 8:1.

### Claim 3 (depends on 1)

The catalyst for methanation reaction as claimed in claim 1, wherein the core consists of cerium dioxide.

### Claim 4 (depends on 1)

The catalyst for methanation reaction as claimed in claim 1, wherein the shell consists of zirconium dioxide.

### Claim 5 (depends on 1)

The catalyst for methanation reaction as claimed in claim 1, wherein the active metal is nickel, rhodium, ruthenium, iridium, platinum, molybdenum, palladium, gold, silver, cobalt, manganese, copper, or a combination thereof.

### Claim 6 (depends on 1)

The catalyst for methanation reaction as claimed in claim 1, wherein an amount of the active metal is 5 wt % to 30 wt %, based on the total weight of the core, shell and active metal.

### Claim 7 (depends on 1)

The catalyst for methanation reaction as claimed in claim 1, wherein the catalyst is spherical-like particle.

### Claim 8 (depends on 1)

The catalyst for methanation reaction as claimed in claim 1, wherein a particle size of the catalyst is 20 nm to 250 nm.

### Claim 9 (depends on 1)

The catalyst for methanation reaction as claimed in claim 1, wherein a particle size of the active metal is 0.1 nm to 30 nm.

### Claim 10 (depends on 1)

The catalyst for methanation reaction as claimed in claim 1, wherein the active metal is nickel, wherein an amount of nickel in the catalyst is 10 atom % to 55 atom %, an amount of cerium in the catalyst is 25 atom % to 75 atom %, and an amount of zirconium is 6 atom % to 36 atom %, wherein a total amount of nickel, cerium and zirconium is 100 atom %.

### Claim 11 (depends on 1)

A method for preparing methane, comprising:
disposing the catalyst as claimed in claim 1 in a continuous reactor; and
introducing a gas into the continuous reactor so that the gas undergoes a hydrogenation in a presence of the catalyst to form methane, wherein the gas comprises hydrogen gas and carbon-oxygen-containing compound.

### Claim 12 (depends on 11)

The method for preparing methane as claimed in claim 11, further comprising:
disposing a catalytic promoter in the continuous reactor
so that the gas undergoes a hydrogenation in a presence of the catalyst and the catalytic promoter to form methane.

### Claim 13 (depends on 12)

The method for preparing methane as claimed in claim 12, wherein the catalytic promoter is lanthanum-containing compound, yttrium-containing compound, gadolinium-containing compound, hafnium-containing compound, samarium-containing compound, neodymium-containing compound, or a combination thereof.

### Claim 14 (depends on 12)

The method for preparing methane as claimed in claim 12, wherein an amount of the catalytic promoter is 0.1 wt % to 10 wt %, based on the total weight of the catalytic promoter and the catalyst.

### Claim 15 (depends on 11)

The method for preparing methane as claimed in claim 11, wherein the continuous reactor is a fixed bed reactor, fluidized bed reactor, or continuous agitated reactor.

### Claim 16 (depends on 11)

The method for preparing methane as claimed in claim 11, wherein the carbon-oxygen-containing compound is carbon monoxide, carbon dioxide, or a combination thereof.

### Claim 17 (depends on 11)

The method for preparing methane as claimed in claim 11, wherein a molar ratio of the hydrogen gas to the carbon-oxygen-containing compound is 3:1 to 10:1.

### Claim 18 (depends on 11)

The method for preparing methane as claimed in claim 11, wherein the hydrogenation has a gas hourly space velocity (GHSV) of 500 hr−1 to 50000 hr−1.

### Claim 19 (depends on 11)

The method for preparing methane as claimed in claim 11, wherein the hydrogenation has a reaction temperature of 180° C. to 400° C.

### Claim 20 (depends on 11)

The method for preparing methane as claimed in claim 11, wherein the hydrogenation has a reaction pressure of 1 kg/cm2 to 20 kg/cm2.