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Porous carbon-supported cobalt-based Fischer-Tropsch synthesis catalyst containing silica additive and preparation method thereof

A silica and catalyst technology, applied in the field of highly active cobalt-based Fischer-Tropsch synthesis catalyst and its preparation, can solve the problem of low catalyst activity and liquid product space-time yield, weak cobalt center and carrier force, and unremarkable reaction effect Significant problems, to achieve the effect of easy large-scale synthesis, high number of specific active sites, and complete reduction

Active Publication Date: 2019-07-16
SOUTH CHINA UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Compared with catalysts based on alumina or silica, cobalt catalysts based on carbon materials have better high-temperature properties, acid and alkali resistance, and better specific surface area. The force is weak, and the cobalt particles are prone to agglomeration behavior during the pretreatment or reaction process and do not meet the optimal size range
Although the preparation methods, compositions and structures of the catalysts reported in each patent and literature are different, and the optimal reaction conditions are also different, the final reaction effect is not particularly remarkable, especially the catalyst activity and the space-time yield of the liquid product are not high. This is mainly due to the unsatisfactory comprehensive factors such as catalyst loading, reduction degree, dispersion, active site particle size, and specific active site density.

Method used

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  • Porous carbon-supported cobalt-based Fischer-Tropsch synthesis catalyst containing silica additive and preparation method thereof
  • Porous carbon-supported cobalt-based Fischer-Tropsch synthesis catalyst containing silica additive and preparation method thereof
  • Porous carbon-supported cobalt-based Fischer-Tropsch synthesis catalyst containing silica additive and preparation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0037] 0.8g cobalt nitrate hexahydrate (Co(NO 3 ) 2 ·6H 2 O) and 0.46g terephthalic acid (H 2 BDC) was placed in a 100mL Shrek tube, and a mixed solution formed by adding 20mL DMF and 5mL absolute ethanol was then used to 2 The air in the tube was replaced by gas and sealed well, heated to 110°C for 15h, then filtered while hot, washed three times with 100mL DMF, and finally dried in air at 100°C for 12h to obtain Co-MOF-71 metal organic framework material.

[0038] A porous carbon-supported cobalt catalyst containing silica was prepared according to the following steps, wherein the molar ratio of cobalt to silica was 5:1. Weigh 0.024g of tetraethyl orthosilicate and place it in 1mL of absolute ethanol to form a mixed solution, impregnate the prepared solution on 0.37g of Co-MOF-71 sacrificial template by conventional impregnation method, and then dry it in air at 65°C After 12 hours, the resulting material was diluted with 3 mL of quartz sand and then placed in a fixed-be...

Embodiment 2

[0042] Using the Co-MOF-71 synthesized in Example 1 as a sacrificial template, a porous carbon-supported cobalt catalyst containing silica was prepared according to the following steps, wherein the molar ratio of cobalt to silica was 5:2. Weigh 0.048g of tetraethyl orthosilicate and place it in 1mL of absolute ethanol to form a mixed solution, impregnate the prepared solution on 0.37g of Co-MOF-71 sacrificial template by conventional impregnation method, and then dry it in air at 65°C After 12 hours, the resulting material was diluted with 3 mL of quartz sand and then placed in a fixed-bed reactor. The temperature was raised to 600 °C at 5 °C / min under He and kept for 8 h, and the molar ratio of cobalt to silicon dioxide was 5:2. Porous carbon-supported cobalt catalyst, the weight of the obtained catalyst is 0.11g, and the volume is about 0.3mL.

[0043] The BET method was used to calculate the specific surface area of ​​the catalyst, and the BJH method was used to calculate t...

Embodiment 3

[0046] Using the synthesized Co-MOF-71 in Example 1 as a sacrificial template, a porous carbon-supported cobalt catalyst containing silica was prepared according to the following steps, wherein the molar ratio of cobalt to silica was 5:3. Weigh 0.072g of tetraethyl orthosilicate and place it in 1mL of absolute ethanol to form a mixed solution, impregnate the prepared solution on 0.37g of Co-MOF-71 sacrificial template by conventional impregnation method, and then dry it in air at 65°C After 12 hours, the resulting material was diluted with 3 mL of quartz sand and then placed in a fixed-bed reactor. The temperature was raised to 600 °C at 5 °C / min under He and kept for 8 h, and the molar ratio of cobalt to silicon dioxide was 5:3. Porous carbon-supported cobalt catalyst, the weight of the obtained catalyst is 0.12g, and the volume is about 0.3mL.

[0047] The BET method was used to calculate the specific surface area of ​​the catalyst, and the BJH method was used to calculate t...

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Abstract

The invention discloses a porous carbon-supported cobalt-based Fischer-Tropsch synthesis catalyst containing silica additives and a preparation method thereof. The catalyst uses cobalt as the active component, silica as the additive, and porous carbon as the carrier. The mass percentage of each component is: cobalt 25.8-30.6%, silica 6.2-21.0%, and the balance is porous carbon carrier. ; The metal cobalt particles on the catalyst are evenly distributed, the particles are densely arranged, the particle diameter is 6 to 9 nm, and there is a silica additive component on the surface of the particles. The present invention uses Co-MOF-71 metal-organic framework as a sacrificial template, adopts an impregnation method to dope silicon source components, and prepares a silica-assisted porous carbon-supported cobalt-based catalyst in a fixed bed through a one-step in-situ pyrolysis method. The catalyst of the invention has a high specific active site density, and when used in Fischer-Tropsch synthesis reaction, it has good C while maintaining high activity. 5+ Selectivity, especially with extremely high C 5+ Space-time yield.

Description

technical field [0001] The invention relates to a cobalt-based Fischer-Tropsch synthesis catalyst, its preparation method and application, in particular to a highly active cobalt-based Fischer-Tropsch synthesis catalyst, its preparation method and application. Background technique [0002] Fischer-Tropsch synthesis refers to the process of hydrogenation of carbon monoxide to generate hydrocarbons and oxygenated compounds. Its main application is to use synthesis gas as raw material to produce chemical products such as gasoline, diesel oil, wax, and liquefied petroleum gas. The product has the characteristics of no sulfur and nitrogen. It is a key step in the indirect conversion of non-petroleum resources such as coal, natural gas or biomass into liquid fuels or chemicals, and has attracted much attention for many years. [0003] Since the Fischer-Tropsch synthesis technology came out in the 1920s, researchers have conducted extensive research on the types of catalysts. A la...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/75B01J35/10C10G2/00
CPCC10G2/332B01J21/08B01J21/18B01J23/75C10G2300/70B01J35/615B01J35/633B01J35/647
Inventor 李映伟裴彦鹏
Owner SOUTH CHINA UNIV OF TECH
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