# US 12,758,951 B2 · Catalyst and method for sulfur-tolerant shift catalytic reaction

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- Number: US 12,758,951 B2
- Document ID: US12758951B2
- Status: Granted
- Kind: B2
- Application number: 18/250,725
- Filed: 2021-09-15
- Published: 2024-07-18
- Granted: 2026-10-13
- Earliest claimed: 2020-10-27
- Assignees: China Petroleum & Chemical Corporation; Sinopec Qilu Company
- Applicants: China Petroleum & Chemical Corporation; Sinopec Qilu Company
- Inventors: Min Wang; Jinshan Xu; Hantao Yu; Zhimin Bai; Hao Wang; Jianbo Jiang; Hongxia Xue
- Web page: https://patentgrep.com/patent/US12758951B2

## CPC

- B01J 23/8871: {Rare earth metals or actinides}
- B01J 21/04: Alumina
- B01J 23/8872: {Alkali or alkaline earth metals}
- B01J 35/613: {10-100 m2/g}
- B01J 37/0236: {Drying, e.g. preparing a suspension, adding a soluble salt and drying}
- B01J 37/035: {Precipitation on carriers}
- B01J 37/036: {to form a gel or a cogel}
- B01J 37/08: Heat treatment {(B01J37/0009, B01J37/0018 take precedence)}
- C01B 3/16: using catalysts
- C01B 2203/0283: containing a CO-shift step, i.e. a water gas shift step
- C01B 2203/1052: Nickel or cobalt catalysts
- C01B 2203/1082: Composition of support materials
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}

## Abstract

A sulfur-tolerant catalyst can be used in the sulfur-tolerant shift catalytic reaction. The catalyst has a carrier and a molybdenum oxide, a cobalt oxide and a cobalt-molybdenum-based perovskite composite oxide carried thereon. The cobalt-molybdenum-based perovskite composite oxide contains a molybdenum element, a cobalt element, an A element, and an oxygen element. The A element is one or more selected from a group consisting of a rare-earth metal element, an alkali metal element and an alkaline earth metal element.

## Claims

### Claim 1

A catalyst comprising a carrier, and a molybdenum oxide, a cobalt oxide and a cobalt-molybdenum-based perovskite composite oxide carried thereon, the cobalt-molybdenum-based perovskite composite oxide comprises a molybdenum element, a cobalt element, an A element, and oxygen;
wherein the A element is one or more selected from rare-earth metal elements, alkali metal elements and alkaline earth metal elements.

### Claim 2 (depends on 1)

The catalyst of claim 1, wherein the A element includes an A1 element being one or more selected from the rare-earth metal elements and an A2 element being one or more selected from alkali metal elements and alkaline earth metal elements.

### Claim 3 (depends on 2)

The catalyst of claim 2, wherein a molar ratio of the A1 element to the A2 element is 1-99: 99-1.

### Claim 4 (depends on 3)

The catalyst of claim 3, wherein a molar ratio of the A1 element to the A2 element is 1-9: 9-1.

### Claim 5 (depends on 2)

The catalyst of claim 2, wherein the catalyst exhibits characteristic peaks at 24.9±0.2° (2θ).

### Claim 6 (depends on 5)

The catalyst of claim 5, wherein the catalyst exhibits characteristic peaks at 24.9±0.2°, 27.9±0.2°, and 36.2±0.2° (2θ) in the X-Ray Diffraction (XRD) pattern.

### Claim 7 (depends on 2)

The catalyst of claim 2, wherein the A1 element is one or more selected from La, Ce, Nd, and Gd, the A2 element is one or more selected from Na, K, Mg, Ca, and Sr.

### Claim 8 (depends on 1)

The catalyst of claim 1, wherein the catalyst exhibits a characteristic peak at 27.9±0.2° (2θ).

### Claim 9 (depends on 8)

The catalyst of claim 8, wherein the catalyst exhibits characteristic peaks at 24.9±0.2°, 27.9±0.2°, and 36.2±0.2°(2θ) in the X-Ray Diffraction (XRD) pattern.

### Claim 10 (depends on 1)

The catalyst of claim 1, wherein the catalyst has a main reduction peak temperature of 600° C. or more.

### Claim 11 (depends on 10)

The catalyst of claim 10, wherein the catalyst has a main reduction peak temperature within a range of 600-850° C. in the H2-TPR pattern.

### Claim 12 (depends on 1)

The catalyst of claim 1, wherein the A element is one or more selected from La, Ce, Nd, Gd, Na, K, Mg, Ca, and Sr.

### Claim 13 (depends on 1)

The catalyst of claim 1, wherein the catalyst has two or more adsorption-desorption peaks at a temperature of 200° C. or more in a programmed temperature rise sulfidation test.

### Claim 14 (depends on 1)

The catalyst of claim 1, wherein the content of A element in the catalyst is 0.4 mol or more and less than 1 mol, relative to a total of 1 mol of molybdenum and cobalt.

### Claim 15 (depends on 1)

The catalyst of claim 1, wherein the content of molybdenum in the catalyst is more than 0.4 mol and less than 1 mol, relative to a total of 1 mol of molybdenum and cobalt.

### Claim 16 (depends on 1)

The catalyst of claim 1, wherein the carrier is selected from alumina, silica, titanium dioxide, zirconium dioxide, magnesium oxide, nickel oxide, a carbon-based carrier, and mixtures thereof.

### Claim 17 (depends on 1)

The catalyst of claim 1, wherein the catalyst comprises a carrier in an amount of 30-90% by mass.

### Claim 18 (depends on 1)

The catalyst of claim 1, wherein the catalyst has a specific surface area of 40 m2·g−1 or more.

### Claim 19 (depends on 1)

A method for sulfur-tolerant shift catalytic reaction, comprising: contacting CO in a feed gas with water vapor in the presence of the catalyst of claim 1;
wherein the feed gas comprises H2S in an amount of 100 ppm or more.

### Claim 20 (depends on 19)

The method of claim 19, wherein the content of H2S is within a range of 100-1,500 ppm.