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Core-shell catalyst as well as preparation method and application thereof

A core-shell catalyst and catalyst technology, applied in catalyst activation/preparation, catalyst, catalytic reaction, etc., can solve the problems of reducing catalytic activity, methanol selectivity, life limit, etc.

Pending Publication Date: 2021-09-07
石河子市中易连疆新能源有限责任公司 +2
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

During the reaction, the surface structure reorganization and particle growth of the catalyst will affect the active interface, greatly reducing the catalytic activity and methanol selectivity.
Therefore, the life of catalysts for industrial methanol synthesis is also severely limited by thermodynamics

Method used

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  • Core-shell catalyst as well as preparation method and application thereof
  • Core-shell catalyst as well as preparation method and application thereof
  • Core-shell catalyst as well as preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0092] Using 5g copper nitrate trihydrate and 6.2g zinc nitrate hexahydrate as raw materials (Cu / Zn=1:1, molar ratio), 6.5gH 3 BTC is an organic ligand, 80ml dimethylformamide (DMF), 80ml ethanol (EtOH) and 80ml deionized water are used as solvents, the above mixture is transferred to a polytetrafluoroethylene reactor, and CuZnO / HKUST- 1 catalyst precursor. Wherein, the temperature is 110° C., and the time is 12 hours. The solvothermal catalyst was filtered, washed and dried at 400 °C in N 2 Roasting in the atmosphere (80ml / min) for 3h and passing through 5wt%H 2 (The mixed gas is composed of hydrogen and nitrogen) reduction at 220 ° C for 10 h, passivation at room temperature overnight, the organic framework of the catalyst precursor is changed into a core-shell structure coated with Cu / ZnO, and the core-shell catalyst CuZnO / HKUST-1. The catalyst (3.0g) will be further subjected to CO / CO in a liquid-phase slurry-bed reactor and a gas-solid-phase fixed-bed reactor. 2 / H ...

Embodiment 2

[0094] Using 4.1g copper acetate monohydrate and 4.6g zinc acetate dihydrate as raw materials (Cu / Zn=1:1, molar ratio), 6.5gH 3 BTC is the organic ligand, 80ml DMF, 80ml EtOH and 80ml deionized water are used as the solvent, the above mixture is transferred to a polytetrafluoroethylene reactor, and the ZnO / HKUST-1 catalyst precursor is prepared by solvothermal method. Wherein, the temperature is 110° C., and the time is 12 hours. The solvothermal catalyst was filtered, washed and dried at 400 °C in N 2 Roasting in the atmosphere (80ml / min) for 3h and passing through 5wt%H 2 (The mixed gas is composed of hydrogen and nitrogen) reduction at 220 ° C for 10 h, passivation at room temperature overnight, the organic framework of the catalyst precursor is changed into a core-shell structure coated with Cu / ZnO, and the core-shell catalyst CuZnO / HKUST-1-AC. The catalyst (3.0g) will be further subjected to CO / CO in a liquid-phase slurry-bed reactor and a gas-solid-phase fixed-bed re...

Embodiment 3

[0096] Using 6.2g zinc nitrate hexahydrate as raw material, 5.2g H 2 BDC was the organic ligand, 80ml DMF was the solvent, and the MOF-5 catalyst precursor was prepared by solvothermal method. Wherein, the temperature is 110° C., and the time is 12 hours. The above mixture was transferred to a polytetrafluoroethylene reactor, and the MOF-5 catalyst precursor was prepared by a solvothermal method. After the solvothermal catalyst was filtered, washed and dried, 5g of copper nitrate trihydrate (Cu / Zn=1:1, molar ratio) was used as raw material, dissolved in 50ml of deionized water, and the catalyst precursor was prepared by ultrasonic-assisted excessive impregnation method Bulk Cu / MOF-5. at 400°C in N 2 Roasting in the atmosphere (80ml / min) for 3h and passing through 5wt%H 2 (The mixed gas is composed of hydrogen and nitrogen) Reduction at 220 °C for 10 h, passivation at room temperature overnight, the organic framework of the catalyst precursor becomes a core-shell structure ...

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Abstract

The invention discloses a core-shell catalyst. The core-shell catalyst comprises MOFs, an active component and an auxiliary agent, wherein the active component and the auxiliary agent coats pore channels and cavities of the MOFs; the active component comprises a Cu element; the auxiliary agent component comprises at least one of a Zn element and a Cr element. The invention also discloses a preparation method and application of the core-shell catalyst. The core-shell catalyst provided by the invention has the characteristics of high dispersity and high specific surface area, is used for CO / CO2 / H2 low-temperature methanol synthesis reaction, and has the advantages of high CO conversion rate, high methanol selectivity, long catalyst life, mild reaction conditions and the like.

Description

technical field [0001] The application relates to a core-shell catalyst, its preparation method and application, and belongs to the field of catalysts. Background technique [0002] Methanol is a basic chemical product widely used as a transportation fuel and a high-energy material for fuel cells, which can be 2 Syngas is produced, and the global annual output is 30-40 million tons. Traditional methanol synthesis using Cu / ZnO / Al 2 o 3 Catalyst, under the reaction conditions of 250-300°C and 50-100bar, the reaction exotherm is severe. In a commercial process, the one-step conversion rate of the reaction gas is only 15-25% due to the limitation of thermodynamic effects. A lower reaction conversion rate will greatly increase the reaction cost, such as the recovery of reaction gas and the loss of equipment. Therefore, the efficiency of industrial methanol synthesis is severely inhibited by thermodynamics. In addition, it is often used by CO / H 2 For the Cu / ZnO catalyst for...

Claims

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Application Information

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IPC IPC(8): B01J31/22B01J31/28B01J31/26B01J35/10B01J37/08B01J37/18C07C29/153C07C29/154C07C31/04
CPCB01J31/1691B01J31/2239B01J31/1815B01J31/28B01J31/26B01J37/08B01J37/18C07C29/153C07C29/154B01J2531/0213B01J2531/16B01J2531/26B01J2231/62B01J2231/625C07C2531/28C07C2531/26C07C2531/22B01J35/615B01J35/647C07C31/04Y02P20/52
Inventor 椿范立宋晓玲周军殷双杰余显军张立张永龙李进
Owner 石河子市中易连疆新能源有限责任公司
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