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Porous carbon loaded double-crystalline phase cobalt-based fischer-tropsch symthesis catalyst and preparation method and application thereof

A cobalt-based, porous carbon technology, applied in chemical instruments and methods, preparation of liquid hydrocarbon mixtures, catalysts for physical/chemical processes, etc. The effect of low temperature and reduced design requirements

Active Publication Date: 2016-11-23
SOUTH CHINA UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Although the porous carbon-supported cobalt catalyst obtained by the pyrolysis of metal-organic frameworks overcomes the problem that cobalt cannot be completely reduced on traditional catalysts, the cobalt on the pyrolyzed material is in a metallic state and will be oxidized and lose its activity when exposed to air. , and cobalt has only one FCC crystal phase, which limits the application of this type of catalyst

Method used

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  • Porous carbon loaded double-crystalline phase cobalt-based fischer-tropsch symthesis catalyst and preparation method and application thereof
  • Porous carbon loaded double-crystalline phase cobalt-based fischer-tropsch symthesis catalyst and preparation method and application thereof
  • Porous carbon loaded double-crystalline phase cobalt-based fischer-tropsch symthesis catalyst and preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0035] 0.8g cobalt nitrate hexahydrate (Co(NO 3 ) 2 ·6H 2 O) and 0.46g terephthalic acid (H 2 BDC) is placed in a 100mL Shrek tube, add a mixed solution formed by 20mL DMF and 5mL absolute ethanol, and then use N 2 The air in the tube was replaced with 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 6h to obtain Co-MOF-71 metal organic framework material.

[0036] 1.48g Co-MOF-71 was placed in a fixed-bed stainless steel reactor, and in a He atmosphere, the temperature was raised to 500°C at a heating rate of 5°C / min for in-situ pyrolysis for 4 hours to obtain a porous carbon-supported cobalt metal intermediate material. Then cool down to room temperature, cut into pure CO gas, the flow rate is 30mL / min, increase the pressure to 2MPa, raise the temperature to 250°C at a heating rate of 5°C / min, keep it for 120h, then cool down to room temperature, use a flow rate of 10mL / min 1 %...

Embodiment 2

[0040] 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 Gas replaced the air in the tube and sealed it well, raised the temperature to 100°C for 10h, then filtered it while it was hot, washed it three times with 100mL DMF, and finally dried it in air at 80°C for 12h to obtain Co-MOF-71 metal-organic framework material.

[0041] 1.48g Co-MOF-71 was placed in a fixed bed reactor, and in a He atmosphere, the temperature was raised to 500°C at a heating rate of 1°C / min for in-situ pyrolysis for 8h to obtain a porous carbon-supported cobalt metal intermediate material, and then Cool down to room temperature, cut into pure CO gas, the flow rate is 30mL / min, increase the pressure to 2MPa, raise the temperature to 250°C at a heating rate of 5°C / min, keep it for 140h, then cool down to room temperature, use a flow rat...

Embodiment 3

[0045] Using the Co-MOF-71 synthesized in Example 1 as a sacrificial template, place 1.48g of Co-MOF-71 in a fixed-bed reactor, and raise the temperature to 550°C at a heating rate of 1°C / min in a He atmosphere In situ pyrolysis for 8 hours to obtain a porous carbon-supported cobalt metal intermediate material, then cooled to room temperature, cut into pure CO gas, the flow rate was 30mL / min, the pressure was increased to 3MPa, and the temperature was raised to 250°C at a heating rate of 5°C / min. Keep for 120h to obtain a porous carbon-supported cobalt carbide intermediate material;

[0046] Take 0.1g porous carbon-supported cobalt carbide intermediate material in H 2 In the atmosphere, the temperature was raised to 450°C at a heating rate of 5°C / min, and kept for 4 hours to obtain a porous carbon-supported bicrystalline cobalt metal catalyst. The mass percentage of cobalt in this material was 30.1% by atomic absorption spectroscopy (AAS). The reaction conditions of the catal...

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Abstract

The invention discloses a porous carbon loaded double-crystalline phase cobalt-based fischer-tropsch symthesis catalyst and preparation method and application thereof. The catalyst takes cobalt as an active component, porous carbon as a carrier and FCC and HCP crystalline phase cobalt as active phases, the mass content of the cobalt is 29.0%-30.8%, and the mass ratio of the HCP crystalline phase to FCC crystalline phase of the cobalt is 0.42-0.97:1. During preparation, a cobalt-contained metal organic skeleton is taken as a sacrificial template which is pyrolyzed under inert atmosphere, porous carbon loaded cobalt carbide intermediates by adopting carbonization of carbon monoxide, and a catalyst precursor is obtained by gas passivation treatment; the catalyst is obtained after the precursor is subjected to hydrogenation activation treatment. The cobalt metal active phases include the FCC and HCP crystalline phases which is high in activity and good in C5+selectivity when used in fischer-tropsch synthesis reaction, high C5+space time yield is specifically achieved, and C5+products are mainly composed of gasoline and diesel compositions.

Description

technical field [0001] The invention relates to a cobalt-based Fischer-Tropsch synthesis catalyst, its preparation method and application, in particular to a porous carbon-supported twin-phase cobalt-based Fischer-Tropsch synthesis catalyst, its preparation method and application. Background technique [0002] Fischer-Tropsch synthesis refers to the process of carbon monoxide hydrogenation reaction to generate hydrocarbons and oxygenated compounds under the action of a catalyst. It is the indirect conversion of non-petroleum resources such as coal, natural gas or biomass into gasoline, A key step in liquid fuels or chemicals such as diesel, wax, and liquefied petroleum gas, it has been a research hotspot in the field of new energy chemical industry 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 large number of experimental studies have proved that the m...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/75B01J35/10C10G2/00
CPCB01J21/18B01J23/75C10G2/332C10G2300/70
Inventor 李映伟裴彦鹏
Owner SOUTH CHINA UNIV OF TECH
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