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Preparation method of hydrophobic carbon-coated iron-based catalyst for Fischer-Tropsch synthesis reaction

An iron-based catalyst, Fischer-Tropsch synthesis technology, which is used in the preparation of liquid hydrocarbon mixtures, chemical instruments and methods, physical/chemical process catalysts, etc., and can solve the problem of low target product selectivity, reduced olefin selectivity, and poor activity and stability. and other problems, to achieve the effect of inhibiting the water-gas shift reaction, improving the selectivity, and ensuring the activity and stability.

Pending Publication Date: 2021-07-27
LINHUAN COKING +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, the traditional FTS catalysts have the problems of low target product selectivity, poor activity and stability.
On the one hand, FTS is a high-temperature, high-pressure exothermic reaction, and water is the main by-product, which makes the water-gas shift reaction (CO+H 2 O→CO 2 +H 2 ) becomes intense, and a considerable part of the CO in the reaction is converted into CO 2 , while reducing CO selectivity, the produced H 2 It will not only inhibit the C-C coupling reaction, but also promote the termination of the carbon chain, resulting in higher CH 4 Selectivity, and it will cause excessive hydrogenation of olefins that have been produced, reducing the selectivity of olefins
On the other hand, researchers now generally believe that the active phase of FTS is iron carbide, and the water generated in the reaction can easily oxidize it, thereby reducing the activity of the catalyst.

Method used

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  • Preparation method of hydrophobic carbon-coated iron-based catalyst for Fischer-Tropsch synthesis reaction
  • Preparation method of hydrophobic carbon-coated iron-based catalyst for Fischer-Tropsch synthesis reaction
  • Preparation method of hydrophobic carbon-coated iron-based catalyst for Fischer-Tropsch synthesis reaction

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Experimental program
Comparison scheme
Effect test

Embodiment 1

[0028] S1. Dissolve 0.404g Fe(NO3)3.9H2O, 0.332g terephthalic acid, and 0.316g graphene powder in 47.7mL deionized water;

[0029] S2, the above mixed solution was magnetically stirred for 30 minutes to obtain a stable and uniform aqueous solution;

[0030] S3. Put the above-mentioned stable and uniform aqueous solution in a polytetrafluoroethylene-lined stainless steel autoclave for hydrothermal reaction, and set the reaction temperature and reaction time to 220°C and 12h, respectively;

[0031] S4. After the reaction, the system is cooled to room temperature, and the mixture is filtered with Whatman filter paper to remove recrystallized terephthalic acid. Wash the black product with ethanol, centrifuge at 7000rpm for 4min, and repeat the operation 3 times;

[0032] S5. Treat the solid sample in ethanol at 80° C. for 4 hours. The precipitate was then centrifuged at 9000 rpm for 20 minutes. Then wash with ethanol and centrifuge at 12000rpm for 15min (in order to ensure that...

Embodiment 2

[0035] S1. Dissolve 0.139g Fe(NO3)3.9H2O, 0.166g isophthalic acid, and 0.458g graphite powder in 77.2mL ethanol;

[0036] S2. The above mixed solution was mechanically stirred by ultrasonic vibration for 30 minutes to obtain a stable and uniform solution;

[0037] S3. Put the above-mentioned stable and uniform aqueous solution in a polytetrafluoroethylene-lined stainless steel autoclave for hydrothermal reaction, and set the reaction temperature and reaction time to 180° C. and 20 h, respectively;

[0038] S4. After the reaction, the system is cooled to room temperature, and the mixture is filtered with filter paper to remove recrystallized isophthalic acid. The black product was washed with ethanol, centrifuged at 8000rpm for 6min, and repeated 4 times;

[0039] S5. Treat the solid sample in ethanol at 60° C. for 3 hours. The precipitate was then centrifuged at 8000 rpm for 10 minutes. Then wash with ethanol and centrifuge at 10000rpm for 5 minutes (in order to ensure that...

Embodiment 3

[0042] S1. Dissolve 0.675g FeCl3 6H2O, 0.135g biphenyl dicarboxylic acid, and 1.823g activated carbon powder in 51.2mLDMF;

[0043] S2, the above mixed solution was magnetically stirred for 30 minutes to obtain a stable and uniform solution;

[0044] S3. Put the above-mentioned stable and uniform solution in a polytetrafluoroethylene-lined stainless steel autoclave for hydrothermal reaction, and set the reaction temperature and reaction time at 200°C and 24h, respectively.

[0045] S4. After the reaction, the system is cooled to room temperature, and the mixture is filtered with filter paper to remove recrystallized biphenyldicarboxylic acid. The black product was washed with DMF, centrifuged at 9000rpm for 8min, and repeated 5 times;

[0046] S5. Treat the solid sample in ethanol at 80° C. for 3 hours. The precipitate was then centrifuged at 9000 rpm for 20 minutes. Then wash with ethanol and centrifuge for 15 minutes at 12000rpm (in order to ensure that the final product ...

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Abstract

The invention relates to the technical field of catalysts, in particular to a preparation method of a hydrophobic carbon-coated iron-based catalyst for Fischer-Tropsch synthesis reaction. The preparation method comprises the following steps: preparing a hydrophobic metal organic framework material MIL-101(Fe)@ NPG by using a hydrothermal method in one step, and calcining the material to obtain the hydrophobic carbon-coated iron-based catalyst for the Fischer-Tropsch synthesis reaction. According to the catalyst, water generated in the Fischer-Tropsch synthesis reaction can be effectively prevented from entering the catalyst, so water-gas shift reaction is inhibited, the generation of C1 byproducts (carbon dioxide and methane) is remarkably inhibited, the selectivity of target hydrocarbon products is improved, an active phase in the catalyst is prevented from being oxidized, and the activity and stability of the catalyst are ensured. The preparation method is simple and easy to operate, good in repeatability, adopts simple, easily available and cheap raw materials and is suitable for large-scale production.

Description

technical field [0001] The invention relates to a hydrophobic Fe@NPG catalyst and its preparation method and its application in Fischer-Tropsch synthesis reaction, belonging to the technical field of catalysts. Background technique [0002] Fischer-Tropsch synthesis is the synthesis of synthesis gas (H from various non-petroleum carbon resources) 2 and CO mixture) into various hydrocarbons and other chemicals under the action of a catalyst. [0003] The main active components of Fischer-Tropsch synthesis are Group VIII metals such as Fe, Co, Ni, Ru, and Pd. Compared with other metal-based catalysts, iron-based Fischer-Tropsch synthesis catalysts have the advantages of low cost, strong poison resistance, and wide reaction conditions. However, the traditional FTS catalysts have the problems of low target product selectivity, poor activity and stability. On the one hand, FTS is a high-temperature, high-pressure exothermic reaction, and water is the main by-product, which mak...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/745C10G2/00
CPCB01J23/745C10G2/332C10G2300/1022B01J35/396
Inventor 刘凯刘建军孟影子魏宇学郭立升薛照明孙松
Owner LINHUAN COKING