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Catalyst for selective pressurized oxidation of methone to prepare C2-C4 olefine and its prepn.

A C2-C4, catalyst technology, applied in the direction of condensation hydrocarbon production with dehydrocarbons, etc., can solve the problems of catalytic activity and selectivity reduction, and achieve improved methane conversion rate, high active component content, and good stability Effect

Inactive Publication Date: 2005-01-12
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

Catalytic activity and selectivity decrease significantly under pressurized conditions

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0012] Embodiment 1: 3.0ml Mn (NO 3 ) 2 (50%), 1.75g ​​Na 2 WO 4 , 1.62gCe 2 (NO 3 ) 3 ·6H 2 O was diluted with 70ml of distilled water, heated to 80°C and added to 35g of SiO that had been heated to 80°C while stirring 2 (40-60 mesh). Before impregnating each active component, SiO 2 are dried, and the impregnated SiO 2 Bake in an oven at 110°C for 16 hours, transfer to a muffle furnace at 550°C, bake in air for 4 hours, raise the temperature to 850°C and bake for 8 hours to prepare the catalyst. At a temperature of 750°C, a pressure of 0.6MPa, and a space velocity of 100,000h -1 、CH 4 / O 2 =4:1, the catalytic reaction performance data without adding any diluent gas is as follows:

[0013] temperature CH 4 Conversion Product distribution (selectivity%) C 2+

[0014] ℃ Conversion rate% C 2 C 3 C 4 CO 2 CO yield

[0015] %

[0016] 750 37.2 29.4 16.4 28.0 10.6 15.6 27.4

[0017] Temperature Reac...

Embodiment 2

[0023] Embodiment 2: 3.0ml Mn (NO 3 ) 2 (50%), 1.75g ​​Na 2 WO 4 , Diluted with 70ml distilled water, the specific method is the same as Example 1. The difference is that 140ml contains 6.49gCe 2 (NO 3 ) 3 ·6H 2 O solution was impregnated in 35g SiO 2 . The drying and roasting of the catalyst are the same as in Example 1. Implemented in the selective oxidation of methane to C 2 -C 4 The hydrocarbon results are as follows:

[0024] Temperature Pressure Space Velocity CH 4 CH 4 Trans Product Selectivity C 2+

[0025] ℃ MPa x10 5 h -1 / O 2 Yield % % Yield

[0026] C 2+ CO x %

[0027] 700 0.6 1.0 4 27.6 72.2 27.8 19.9

Embodiment 3

[0028] Embodiment 3: measure 4.5ml Mn (NO 3 ) 2 (50%), diluted with 70ml of distilled water, heated to 80°C and added to 35g of SiO that had been heated to 80°C at one time while stirring 2 And dry; use 140ml containing 2.39g Na 2WO 4 The solution was added to the SiO that had been heated to 80°C 2 ; Reuse 210ml containing 12.98g Ce 2 (NO 3 ) 3 ·6H 2 The O solution was added to the SiO that had been heated to 80 °C 2 , drying and roasting are the same as example 1. The catalyst is used in the selective oxidation of methane to C 2 -C 4 The hydrocarbon evaluation results are as follows:

[0029] Temperature Pressure Space Velocity CH 4 CH 4 Trans Product Selectivity C 2+

[0030] ℃ MPa x10 5 h -1 / O 2 Yield % % Yield

[0031] C 2+ CO x %

[0032] 740 0.6 1.0 4 28.1 67.2 32.8 18.9

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PUM

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Abstract

The present invention relates to a multicomponent catalyst using SiO2 as carrier and containing valence-changed metal oxide, alkali metal and rare earth oxide, its active component is formed from Mn2O3, Na2WO4 and SnO2, its content is 10 wt%-20 wt%. Said catalyst can be used for methane selective oxidation reaction to prepare C2-C4 hydrocarbons under the condition of pressurization. Under the condition of having no diluent gas, 0.6 MPa and high space velocity it can obtain 27.4% of C2 hydrocarbon yield, at the same time can obtain lots of C3-C4 hydrocarbons.

Description

technical field [0001] The present invention relates to the production of C by selective oxidation of methane under pressurized conditions 2 -C 4 Hydrocarbon catalysts and methods for their preparation. Background technique [0002] With the continuous increase of proven reserves of natural gas and the increasing scarcity of oil resources, the process of producing high-carbon hydrocarbons through selective oxidation of methane has strong advantages over the traditional tube furnace oil cracking process, which is of great significance to the effective use of natural gas resources , the research on the production of high value-added chemicals using natural gas as raw material is currently a hot topic that is very active and widely concerned at home and abroad. There are a lot of literature and patent reports on catalyst systems in this field, and the catalyst composition covers almost all available elements in the periodic table, most of which are methane oxidative coupling ...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/34C07C2/84
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