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Silica composite doped with metal and/or its oxide in situ and use thereof

A technology of silica and oxides, applied in the direction of hydrocarbon production from carbon oxides, physical/chemical process catalysts, chemical/physical processes, etc., can solve problems such as reduced catalytic activity and poor thermal stability

Active Publication Date: 2017-10-27
EAST CHINA UNIV OF SCI & TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0003] Most of the existing catalysts used to prepare methane from syngas are supported catalysts (that is, the active components of the catalyst are mostly loaded on the corresponding carrier by impregnation method). Although this type of supported catalyst has high catalytic activity and selectivity, However, its thermal stability is not good (that is, under high temperature (such as 500 ° C ~ 700 ° C) conditions, the catalytic activity of this type of supported catalyst will decrease), and needs to be improved

Method used

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  • Silica composite doped with metal and/or its oxide in situ and use thereof
  • Silica composite doped with metal and/or its oxide in situ and use thereof
  • Silica composite doped with metal and/or its oxide in situ and use thereof

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preparation example Construction

[0030] The method for preparing the silicon dioxide compound doped with metal or / and its oxide as described above in the present invention specifically includes the following steps:

[0031] (1) Prepare a nickel salt solution with a mass percentage concentration of 1wt% to 20wt%, a mass percentage of a rare earth metal salt solution with a mass percentage of 0wt% to 5wt%, a mass percentage of a "rare metal" salt solution with a mass percentage of 0wt% to 10wt%, and the mass The percentage is 0wt%~5wt% alkali metal salt solution;

[0032] (2) First, place the template agent, "alkali source" and "silicon source" in the reactor at room temperature (20°C ~ 40°C, the same below) and under stirring conditions, and continue stirring for 0.5 hours to After 24 hours, add the "metal source" solution dropwise and continue to stir for 0.5 to 24 hours to obtain an emulsion; finally, react the obtained emulsion with hydrothermal reaction at 80°C to 180°C for 12 to 100 hours, and quench to ...

Embodiment 1

[0049] Weigh 2.428 g of cetyltrimethylammonium bromide (template) and dissolve it in deionized water at 40°C to obtain an aqueous template solution. Weigh 1.619g of nickel nitrate hexahydrate and dissolve it in 20ml of deionized water to prepare an aqueous solution of nickel nitrate. Dissolve 0.447g NaOH in 10ml deionized water to obtain NaOH aqueous solution.

[0050] The obtained NaOH aqueous solution was slowly dropped into the above-mentioned template aqueous solution under vigorous stirring. Under vigorous stirring, 11.565 g of ethyl orthosilicate was added dropwise into the aqueous template solution. After the dropwise addition, stir vigorously for 2h, then start to slowly add nickel nitrate aqueous solution dropwise, after the dropwise addition, stir vigorously at room temperature for 2h, move the product to a hydrothermal reaction kettle, and crystallize at 120°C for 72h. Then it was rapidly cooled to room temperature, filtered, and the filter cake was washed until n...

Embodiment 2

[0054] Replace the nickel nitrate in embodiment 1 with lanthanum nitrate and nickel nitrate, obtain the metal nickel of doping 10wt% or / and its oxide compound and the metal lanthanum of doping 1wt% or / and its oxide with similar method in embodiment 1 compound of silica (abbreviated as catalyst B).

[0055] Catalyst evaluation method is identical with embodiment 1, and catalyst B is under 1.5Mpa, space velocity 12000h -1 , the conversion rate of carbon monoxide is 100%, and the selectivity of methane is over 99%.

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Abstract

The invention relates to a silicon dioxide compound doped with metal and / or its oxide in situ and its application. The silicon dioxide composite is obtained by in-situ doping of metal or / and its oxide and by hydrothermal synthesis, and the specific surface area (BET) of the target is 100m2 / g-800m2 / g. Based on the total weight of the silicon dioxide compound doped with metal or / and its oxide as 100wt%, the doping amount of metal nickel or / and its oxide is 1wt%~20wt%, and the rare earth metal or / and The doping amount of its oxide is 0wt%~5wt%, the doping amount of "rare metal" or / and its oxide is 0wt%~10wt%; the doping amount of alkali metal or / and its oxide is 0wt% ~5wt%, the balance is silica. The application of the silicon dioxide compound doped with metal or / and its oxide as a catalyst for the reaction of preparing methane from synthesis gas provided by the invention.

Description

technical field [0001] The invention relates to a silicon dioxide compound doped with metal and / or its oxide in situ and its application. Background technique [0002] The methanation of synthesis gas is one of the main reactions of coal to natural gas, which is a strong exothermic reaction, which will lead to a large increase in the temperature of the reaction gas, and easily cause the sintering of the active components of the catalyst. Therefore, an excellent catalyst for syngas methanation needs to have high catalytic activity and selectivity at "low temperature" (such as 300°C-400°C); and maintain good thermal stability at high temperature (such as 500°C-700°C). Stability (mainly manifested as no reduction in catalytic activity). [0003] Most of the existing catalysts used to prepare methane from synthesis gas are supported catalysts (that is, the active components of the catalyst are mostly supported on the corresponding carrier by impregnation method). Although this ...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J29/76B01J29/78B01J23/755B01J23/83B01J23/887C07C9/04C07C1/04
Inventor 辛忠张加赢
Owner EAST CHINA UNIV OF SCI & TECH
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