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Methane oxidative coupling catalyst, preparation method thereof and method for preparing C2 hydrocarbon by oxidative coupling of methane

An oxidative coupling and catalyst technology, applied in metal/metal oxide/metal hydroxide catalysts, heterogeneous catalyst chemical elements, physical/chemical process catalysts, etc., can solve the problem of insufficient catalytic activity and product selectivity, The preparation method is complex and other problems, to achieve high industrial application prospects, simple steps, and the effect of improving the conversion rate

Pending Publication Date: 2021-06-11
CHINA PETROLEUM & CHEM CORP +1
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  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0006] Oxidative coupling of methane is an exothermic reaction, and the reaction temperature is usually 750-850°C or higher, which requires the catalyst to be stable at high temperature in order to achieve high catalytic activity and product selectivity. However, the catalytic activity and product selectivity are still not high enough, and the preparation method is complicated, which have become important factors restricting the industrialization of methane oxidative coupling reaction.

Method used

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  • Methane oxidative coupling catalyst, preparation method thereof and method for preparing C2 hydrocarbon by oxidative coupling of methane

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preparation example Construction

[0021] According to the second aspect of the present invention, the present invention provides a method for preparing a methane oxidative coupling catalyst, the preparation method comprising: in the presence of water, sodium tungstate, soluble salts of erbium, soluble salts of manganese and square The quartz is contacted, dried and calcined, so that the oxides of sodium tungstate, erbium oxide and manganese are supported on the cristobalite.

[0022] According to the preparation method of the present invention, the consumption of sodium tungstate, the soluble salt of erbium, the soluble salt of manganese and cristobalite make in the prepared catalyst, based on the weight of cristobalite, the content of sodium tungstate is 1-15% by weight, The content of erbium oxide is 0.01-10% by weight, and the content of manganese oxide is 0.1-6.5% by weight in terms of manganese.

[0023] According to the preparation method of the present invention, the consumption of sodium tungstate, the...

Embodiment approach

[0029] According to another specific embodiment, the preparation method of the catalyst comprises the following steps:

[0030] (1) In the presence of water, the aqueous solution of manganese-containing soluble salt and sodium tungstate is contacted with cristobalite, and then dried to obtain cristobalite impregnated with manganese and sodium tungstate;

[0031] (2) The cristobalite impregnated with manganese and sodium tungstate is brought into contact with the erbium soluble salt solution, followed by drying and firing.

[0032] In step (1), the cristobalite can be impregnated with an aqueous solution of a soluble salt of manganese and an aqueous solution of sodium tungstate, respectively, or can be impregnated with an aqueous solution of a soluble salt of manganese and sodium tungstate at the same time. The contacting is carried out under stirring, preferably at room temperature (20-45° C.) for 1-2 hours.

[0033] In step (2), the contacting is carried out under stirring, ...

Embodiment 1

[0050] (1) Preparation of aqueous solution for impregnation

[0051] 4.68 g of manganese nitrate solution was dissolved in 20 mL of water to obtain manganese nitrate aqueous solution. Dissolve 0.67 g of sodium tungstate dihydrate in 20 mL of water to obtain an aqueous solution of sodium tungstate. Dissolve 0.014 g of erbium nitrate pentahydrate in 20 mL of water to obtain an erbium nitrate solution.

[0052] (2) Preparation of catalyst

[0053] Add 12g of cristobalite carrier to manganese nitrate aqueous solution, stir at room temperature for 1h, and then dry at 120°C for 2h after rotary evaporation at 80°C for 3h to obtain manganese-impregnated carrier; then add sodium tungstate aqueous solution, stir at room temperature for 1h, After rotary evaporation for 2 hours, dry at 120°C for 2 hours to obtain a carrier impregnated with manganese and sodium tungstate; finally add erbium nitrate aqueous solution, stir at 50°C for 1 hour, rotate at 80°C for 3 hours, dry at 120°C for 2 ...

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Abstract

The invention relates to the field of comprehensive utilization of natural gas, and discloses a methane oxidative coupling catalyst, a preparation method thereof and a method for preparing C2 hydrocarbon by oxidative coupling of methane. The catalyst comprises cristobalite and an active component loaded on the cristobalite; the active component comprises sodium tungstate, erbium oxide and manganese oxide; and in the catalyst, based on the weight of cristobalite, the content of sodium tungstate is 1-15 wt%, the content of erbium oxide is 0.01-10 wt%, and the content of manganese oxide is 0.1-6.5 wt% in terms of manganese. The catalyst provided by the invention can promote the proceeding of methane coupling oxidation reaction, and improve the conversion rate of methane and the yields of ethylene and ethane.

Description

technical field [0001] The invention relates to the comprehensive utilization of natural gas, in particular to a methane oxidative coupling catalyst, a preparation method thereof, and a method for producing carbon dihydrocarbons through methane oxidative coupling. Background technique [0002] Ethylene is the most important basic organic chemical raw material. Its production has long depended on the petroleum cracking process, and the resulting environmental pollution has become increasingly serious. Furthermore, the price of crude oil has continued to rise in recent years, leading to an increase in the price of ethylene cracking raw materials, and the supply of ethylene cracking raw materials is in short supply. Faced with this situation, all countries in the world are adjusting the energy utilization structure and constantly looking for new ethylene production routes. Natural gas is an important energy source, and its abundant reserves provide a good guarantee for its uti...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/34C07C2/84C07C9/06C07C11/04
CPCB01J23/34B01J23/002C07C2/84B01J2523/00Y02P20/52
Inventor 武洁花张明森冯静刘东兵
Owner CHINA PETROLEUM & CHEM CORP
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