Catalyst for pressurized oxidative coupling of methane to prepare ethylene and its prepn.

An oxidative coupling and catalyst technology, applied in physical/chemical process catalysts, metal/metal oxide/metal hydroxide catalysts, chemical instruments and methods, etc., can solve the problem of increasing reaction pressure, catalytic activity and selectivity decline , unfavorable operation and other problems, to achieve the effect of high content of active components

Inactive Publication Date: 2003-01-08
LANZHOU INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, after the reaction pressure is increased, the catalytic activity and selectivity of the existing catalyst system will decrease, which is not conducive to operation under pressurized conditions.

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0012] Embodiment 1: measure 1ml Mn (NO 3 ) 2 (50%wt), diluted with 20ml of distilled water, heated to 80°C and added to 10.5g of SiO that had been heated to 80°C while stirring 2 , dried at 110°C; weighed 0.53g Na 2 WO 4 Dissolve in 20ml of distilled water, heat to 80°C and add to SiO that has been heated to 80°C while stirring 2 And dry; Weigh 3.38g of dibutyltin dilaurate and dissolve in 20ml of methanol, stir and add to SiO which has been heated to 80°C 2 , baked in an oven at 110°C for 16 hours, transferred to a muffler furnace at 550°C, baked in air for 4 hours, raised the temperature to 850°C and baked for 8 hours to prepare the catalyst. The catalytic performance data of the catalyst are as follows:

[0013] Catalyst Temperature Pressure Methane Stream CH 4 / CH 4 Turn to C 2+ Choose C 2+ receive

[0014] Loading g ℃ MPa Velocity L / h O 2 Conversion rate% Selectivity% Rate%

[0015] 0.4 700 0.6 0.78 4 25.5 60.8 15.5

[0016] 0.4 750 0.6 0.78 4 31.6 71....

Embodiment 2

[0022] Embodiment 2: get 3.0ml Mn (NO 3 ) 2 (50%wt), 1.59g Na 2 WO 4 , diluted with 40ml distilled water, impregnated in 31.5g SiO 2 Above, the method is the same as Example 1. Then use 40ml of toluene solution containing 8.32g dibutyltin dilaurate to impregnate SiO 2 superior. The drying and roasting of the catalyst are the same as in Example 1. Implemented in methane oxidative coupling results are as follows:

[0023] Catalyst Loading Temperature Pressure Methane Flow CH 4 CH 4 C 2+ Choose C 2+ receive

[0024] g ℃ MPa Velocity L / h / O 2 Conversion selectivity %

[0025] Rate% %

[0026] 0.4 730 0.6 0.89 8 20.0 75.5 15.1

Embodiment 3

[0027] Embodiment 3: get 1.0ml Mn (NO 3 ) 2 (50%wt), 0.53g Na 2 WO 4 , diluted with 20ml distilled water, impregnated in 10.5g SiO 2 Above, the method is the same as Example 1. When impregnating the active component Sn, 20ml containing 1.54g SnSO 4 10% methanol in water. The drying and roasting of the catalyst are the same as in Example 1. The evaluation results for methane oxidative coupling are as follows:

[0028] Catalyst Loading Temperature Pressure Methane Flow CH 4 CH 4 C 2+ Choose C 2+ receive

[0029] g ℃ MPa Velocity L / h / O 2 Conversion selectivity %

[0030] Rate% %

[0031] 0.4 720 0.6 1.11 4 30.2 61.3 18.5

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Abstract

The present invention discloses a catalyst for methane oxidative coupling polymerization to prepare ethylene under the condition of pressurization, and said catalyst uses SiO2 as support, and its active component is formed from Mn2O3, Na2WO4 and SnO2, and its active component content is 10 wt%-20 wt%. Under the condition of no dilution gas, 0.6 MPa and high space velocity it can obtain 33.0% of methane conversion rate and 24.1% of C2 hydrocarbon yield.

Description

technical field [0001] The invention relates to a catalyst for ethylene oxidative coupling reaction under pressure and a preparation method thereof. Background technique [0002] The process of oxidative coupling of methane to ethylene is one of the most important directions of direct conversion of natural gas. At present, the research at home and abroad is very active and has attracted widespread attention. There are many literatures and patent reports related to methane oxidative coupling catalyst systems, and there are more than a thousand kinds of catalysts, most of which are catalyst systems under normal pressure conditions. However, few catalysts have been developed for the oxidative coupling of methane under pressure. Aika once published an article in Journal of Catalysis (J.Catal.1999, 181, 160) and reported SnO 2 - Li / MgO methane oxidative coupling catalyst. ZL 91104243.1 discloses a catalyst for the selective oxidation of methane to ethylene containing alkali me...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/34C07C2/84
CPCY02P20/52
Inventor 丑凌军李树本蔡迎春张兵牛建中季生福赵军
Owner LANZHOU INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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