Catalyst for preparing ethylene through oxidative coupling of methane, preparation method of catalyst and method for preparing ethylene through oxidative coupling of methane
A technology of oxidative coupling and catalyst, applied in the direction of metal/metal oxide/metal hydroxide catalyst, physical/chemical process catalyst, chemical instrument and method, etc., can solve the problems of low catalytic activity, low selectivity of higher hydrocarbons, The ethylene content needs to be improved to achieve high catalytic activity, increase content and yield, and promote the effect of methane oxidative coupling reaction
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[0022] In a second aspect, the present invention provides a method for preparing a catalyst for oxidative coupling of methane to ethylene, the preparation method comprising:
[0023] (1) In the presence of water, contact amorphous silicon dioxide with ammonium tungstate and sodium hydroxide, dry and roast to obtain cristobalite containing sodium tungstate and silicon dioxide;
[0024] (2) In the presence of water, the cristobalite is contacted with a soluble salt of samarium, a soluble salt of manganese and optional sodium tungstate, dried and roasted;
[0025] In step (1), relative to 100 parts by weight of amorphous silica, the total amount of ammonium tungstate and sodium hydroxide is 0.008-5 parts by weight, preferably 0.01-4 parts by weight; ammonium tungstate and sodium hydroxide The molar ratio of the amount used is 1: (1-3). It should be understood that the ammonium tungstate used to prepare cristobalite usually exists in the form of its hydrate.
[0026] According t...
Embodiment approach
[0038] According to a specific implementation manner, step (2) includes:
[0039] S1: contacting the cristobalite with an aqueous solution of manganese-containing soluble salt and optional sodium tungstate, and then drying to obtain cristobalite impregnated with manganese and optional sodium tungstate;
[0040] S2: contacting the manganese-impregnated cristobalite with samarium soluble saline solution, followed by drying and calcining.
[0041] In this embodiment, in step S1, in the case that sodium tungstate needs to be additionally loaded on the carrier, the carrier can be impregnated with an aqueous solution containing the manganese-containing soluble salt and sodium tungstate; The aqueous solution of soluble salt and the aqueous solution of sodium tungstate impregnate the carrier respectively. In the aqueous solution, the concentration of the soluble manganese salt can be, for example, 1-15% by weight, and the concentration of sodium tungstate can be, for example, 2-10% b...
Embodiment 1
[0060] (1) Dissolve 3.6g of ammonium tungstate pentahydrate and 0.4g of sodium hydroxide in 80mL of water, add 80g of amorphous silicon dioxide, stir at room temperature for 1h, remove water by rotary evaporation at 80°C, dry in an oven at 120°C overnight, and then Raise the temperature to 800°C at a rate of 5°C / min in air, and cool to room temperature to obtain cristobalite. The XRD analysis results show that its structure is the characteristic peak of cristobalite (the peak positions are at 20°, 35°, 44°, 56° respectively). It can be seen that cristobalite has been successfully prepared.
[0061] (2) Dissolve 8.13g of manganese nitrate solution in 18mL of water, add 25g of cristobalite, stir at room temperature for 1h, and rotate the stirred product at 80°C for 2h, then dry at 120°C for 2h to obtain manganese-impregnated cristobalite.
[0062] Dissolve 0.028g of sodium tungstate dihydrate in 25mL of water, add cristobalite impregnated with manganese, stir at room temperature...
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