Methane oxidation coupling catalyst and preparation method thereof

A catalyst and methane technology, applied in the direction of catalyst activation/preparation, carbon compound catalyst, catalyst, etc., can solve the problems of easy loss of alkali metal, increased explosion risk, catalyst deactivation, etc., and achieve high thermal and chemical stability, and reaction Good stability and low temperature activity

Active Publication Date: 2015-07-08
ECO ENVIRONMENTAL ENERGY RES INST +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

This kind of catalyst not only has a low product yield, but also the alkali metal is easy to lose and cause the deactivation of the catalyst
[0007] Chinese patent publication CN1068052A discloses an alkaline earth or rare earth metal fluoride as the main component, together with a small amount of alkaline earth or rare earth metal oxide or ThO 2 , ZrO 2 According to the disclosure of this document, the catalyst of this document is applied to the oxidative coupling reaction of methane, and the methane conversion rate of 27-34% can be obtained, but C 2 + The yield of hydrocarbon products is only 13-20%
However, the reaction system needs to be pressurized, which will increase the risk of explosion and pose a safety hazard

Method used

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  • Methane oxidation coupling catalyst and preparation method thereof
  • Methane oxidation coupling catalyst and preparation method thereof
  • Methane oxidation coupling catalyst and preparation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0042] The purpose of this example is to provide 2.8MnO 2 1.0Na 2 O 3.6 WO 3 3.0TiO 2 89.6SiO2 2 Catalyst preparation.

[0043] a) Weigh 0.11 g of sodium tungstate (Na 2 WO 4 2H 2 O) Dissolve in 2.5ml of deionized water to form an aqueous solution of sodium tungstate; weigh 2.00g of dry Ti-MWW molecular sieve (Si / Ti ratio 40) into a 100ml beaker, first add 5.0ml of deionized water to disperse the molecular sieve Finally, add the sodium tungstate aqueous solution prepared above dropwise, ultrasonically disperse for 0.5 hours and then continue to stir for 3 hours to obtain a slurry-like viscous mixture;

[0044] b) Weigh 0.247 g of 50% manganese nitrate aqueous solution, add deionized water to dilute to 2 ml; add the obtained manganese nitrate aqueous solution dropwise to the slurry-like viscous mixture obtained in step a) under stirring, and continue stirring for 3 hours, Dry at 90°C;

[0045] c) The sample prepared in step b) was ground into powder, and calcined at 55...

Embodiment 2

[0048] The purpose of this example is to provide 4.2MnO 2 1.5Na 2 O·5.5WO 3 2.9TiO2 2 ·85.9SiO2 2 Catalyst preparation.

[0049] a) Weigh 0.177 grams of sodium tungstate (Na 2 WO 4 2H 2 O) Dissolve in 2.5ml of deionized water to form an aqueous solution of sodium tungstate; weigh 2.00g of dry Ti-MWW molecular sieve (Si / Ti ratio 40) into a 100ml beaker, first add 5.0ml of deionized water to disperse the molecular sieve Finally, add the sodium tungstate aqueous solution prepared above dropwise, ultrasonically disperse for 1 hour, and then continue stirring for 1 hour to obtain a slurry-like viscous mixture;

[0050] b) Weigh 0.391 g of 50% manganese nitrate aqueous solution, add deionized water to dilute to 2 ml; under stirring, add the obtained manganese nitrate aqueous solution dropwise into the slurry-like viscous mixture obtained in step a), and continue stirring for 1 hour, Dry at 80°C;

[0051] c) The sample prepared in step b) was ground into powder, and calcined...

Embodiment 3

[0054] The purpose of this example is to provide 6.5MnO 2 2.3Na 2 O 8.6 WO 3 2.7TiO2 2 79.9 SiO2 2 Catalyst preparation.

[0055] a) Weigh 0.295 grams of sodium tungstate (Na 2 WO 4 2H 2 O) Dissolve in 2.5ml of deionized water to form an aqueous solution of sodium tungstate; weigh 2.00g of dry Ti-MWW molecular sieve (Si / Ti ratio 40) into a 100ml beaker, first add 5.0ml of deionized water to disperse the molecular sieve Finally, add the sodium tungstate aqueous solution prepared above dropwise, ultrasonically disperse for 0.5 hours, and then continue to stir for 2 hours to obtain a slurry-like viscous mixture;

[0056] b) Weigh 0.651 g of 50% manganese nitrate aqueous solution, add deionized water to dilute to 2 ml; under stirring, add the obtained manganese nitrate aqueous solution dropwise into the slurry-like viscous mixture obtained in step a), and continue stirring for 3 hours, Dry at 100°C;

[0057] c) The sample prepared in step b) was ground into powder, and ca...

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PUM

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Abstract

The present invention discloses a manganese-sodium-tungsten-silicon composite oxide oxidative coupling of methane catalyst containing or not containing titanium, obtained by loading manganese-sodium-tungsten onto a titanium-silicon molecular sieve or a pure silicon molecular sieve by means of a step-by-step impregnation method and calcination. The manganese-sodium-tungsten-silicon composite oxide catalyst containing or not containing titanium has the following structural formula: vMnO2·xNa2O·yWO3·zTiO2·(100-v-x-y-z)SiO2, the v, x, y, and z respectively representing the fractional quality occupied by metal manganese oxide, sodium oxide, tungsten oxide and titanium oxide, 0.3≤v≤16, 0.1≤x≤5, 0.6≤y≤21, 0.0≤z≤4. The manganese-sodium-tungsten-silicon composite oxide catalyst containing or not containing titanium set forth in the present invention is used for oxidative coupling of methane reactions, having excellent low-temperature catalytic activity and ethylene/propylene selectivity generation and reaction stability.

Description

technical field [0001] The invention relates to a catalyst and a preparation method thereof, in particular to a titanium-containing or titanium-free manganese-sodium-tungsten-silicon composite oxide methane oxidative coupling catalyst and a preparation method thereof. Background technique [0002] Both methane and olefins (such as ethylene) are important chemical raw materials. There are already industrial processes for preparing olefins from methane, such as the Benson method, partial oxidation method and catalytic pyrolysis method (Liaoning Chemical Industry 1 (1985) 11) . In the traditional Benson method, there are by-products of chlorinated hydrocarbons, which cause certain difficulties in separation; in the catalytic pyrolysis method, a large amount of carbon deposits are generated, which seriously affects the stability and service life of the catalyst. [0003] Many existing methods use methane coupling catalysts. Therefore, the development of methane coupling catalys...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/89B01J29/035B01J23/34C07C2/84C07C11/04C07C11/06
CPCB01J23/34B01J21/06B01J23/30B01J23/04C07C2/84B01J21/08B01J37/08B01J37/02B01J23/002B01J29/0358B01J29/89B01J2229/186B01J2523/00C07C2521/06C07C2521/08C07C2523/04C07C2523/30C07C2523/34Y02P20/52C07C11/04C07C11/06B01J2523/12B01J2523/41B01J2523/69B01J2523/72B01J2523/47
Inventor 路勇王郁王鹏伟何鸣元徐彬周晓莹萧锦诚
Owner ECO ENVIRONMENTAL ENERGY RES INST
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