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Catalyst for preparing low-carbon mixed alcohol through carbon oxide hydrogenation and preparation method of catalyst

A technology of low-carbon mixed alcohols and catalysts, applied in the direction of organic compound/hydride/coordination complex catalysts, chemical instruments and methods, metal/metal oxide/metal hydroxide catalysts, etc., can solve the problem of reduction and catalyst preparation Problems such as lengthy steps and difficulty in alcohol separation, to achieve the effect of dense particles, good space-time yield and good selectivity

Inactive Publication Date: 2017-07-25
NINGXIA UNIVERSITY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Chinese patent CN 105582970 A reports a SiO 2 or Al 2 o 3 Loaded Co 2 C and Co catalysts, although the distribution of methanol in the total alcohols of the catalyst system is lower than that of the above four systems, the preparation steps of the catalyst are lengthy, and alcohols with a carbon chain length greater than 6 carbon numbers are generated, which leads to the formation of alcohols. Difficulty separating

Method used

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  • Catalyst for preparing low-carbon mixed alcohol through carbon oxide hydrogenation and preparation method of catalyst
  • Catalyst for preparing low-carbon mixed alcohol through carbon oxide hydrogenation and preparation method of catalyst
  • Catalyst for preparing low-carbon mixed alcohol through carbon oxide hydrogenation and preparation method of catalyst

Examples

Experimental program
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Effect test

Embodiment 1

[0034] 0.8g cobalt nitrate hexahydrate (Co(NO 3 ) 2 ·6H 2 O) and 0.46g terephthalic acid (H 2 BDC) was placed in a 150mL Shrek tube, and a mixed solution formed by adding 20mL N,N-dimethylformamide and 5mL absolute ethanol was added, sealed and heated to 110°C for 15h, then filtered while hot, and 100mL N,N- DMF was washed three times, and finally dried in air at 100° C. for 6 h to obtain Co-MOF-71 metal-organic framework material.

[0035] 1.48g Co-MOF-71 was placed in a fixed-bed stainless steel reactor, and heated to 500°C for 8 hours in an Ar atmosphere at a heating rate of 5°C / min to obtain a carbon-supported Co intermediate material. The mass percentage of Co element in this material was determined to be 27.0% by atomic absorption spectroscopy (AAS). After the pyrolysis is completed, cool down to room temperature, cut into pure CO gas with a space velocity of 24L / h / g-sample, increase the pressure to 2MPa, raise the temperature to 250°C at a heating rate of 1°C / min, k...

Embodiment 2

[0039] 0.8g cobalt nitrate hexahydrate (Co(NO 3 ) 2 ·6H 2 O) and 0.46g terephthalic acid (H 2 BDC) was placed in a 150mL Shrek tube, a mixed solution formed by adding 40mL N,N-dimethylformamide and 10mL absolute ethanol was added, sealed and heated to 120°C for 12h, then filtered while hot, and 100mL N,N- DMF was washed three times, and finally dried in air at 80° C. for 12 hours to obtain Co-MOF-71 metal-organic framework material.

[0040] 1.48g Co-MOF-71 was placed in a fixed-bed stainless steel reactor, and heated to 600°C for 4 hours in an Ar atmosphere at a heating rate of 1°C / min to obtain a carbon-supported Co intermediate material. The mass percentage content of Co element was determined to be 33.1% by AAS characterization. After the pyrolysis was completed, the temperature was lowered to room temperature, and the pure CO gas with a space velocity of 30L / h / g-sample was cut in, and the pressure was increased to 3MPa. The heating rate was raised to 280 °C, kept for ...

Embodiment 3

[0044] 0.8g cobalt nitrate hexahydrate (Co(NO 3 ) 2 ·6H 2 O) and 0.46g terephthalic acid (H 2 BDC) was placed in a 150mL Shrek tube, and a mixed solution formed by adding 30mL N,N-dimethylformamide and 10mL absolute ethanol was added, sealed and heated to 110°C for 15h, then filtered while hot, and 100mL N,N- DMF was washed three times, and finally dried in air at 80° C. for 12 hours to obtain Co-MOF-71 metal-organic framework material.

[0045] According to the following steps to prepare carbon-supported Co&Co with a mass content of 14.1% silica additives 2 Catalyst C: Weigh 0.070g of tetraethyl orthosilicate and place it in 1.58g of absolute ethanol to form a mixed solution, add 0.37g of Co-MOF-71, stir at room temperature for 10min, then add 0.1g of ammonia water, and then in air at 80°C After drying for 12 hours, the obtained material was then placed in a fixed-bed reactor, and the temperature was raised to 500°C under Ar at 5°C / min and kept for 8h. The mass percentage...

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Abstract

The invention relates to a catalyst for preparing low-carbon mixed alcohol and liquid hydrocarbon through catalytic conversion of a synthesis gas and a preparation method of the catalyst. The catalyst is prepared from a carrier, an active component and an assistant, wherein the carrier is carbon; the active component is nanocomposite particles of metal Co and cobalt carbide Co2C; the assistant is SiO2; and the mass content of Co is 0.4-2.1wt%, the mass content of the Co2C is 37.7-42.0%, the mass content of the SiO2 is 0-14.3% and the balance is carbon. The preparation method of the catalyst comprises the following steps of (1) preparing a Co-MOF-71 organic metal skeleton material; (2) adopting Co-MOF-71 as a sacrificial template and tetraethylortho silicate as a silicon source and preparing a catalyst precursor containing a Si element in situ; and (3) activating the catalyst precursor to obtain a carbon-supported Co&Co2C catalyst containing the SiO2 assistant. The preparation method is simple, the nanocomposite particles are formed through the Co and the Co2C, distribution of alcohol is narrow and the space-time yield of the alcohol is good. The SiO2 assistant is distributed on the surfaces of the active component particles of the catalyst in an embedded form and plays a relatively good synergistic effect on the catalytic activity.

Description

technical field [0001] The invention relates to a technology for catalytic conversion of synthetic gas to liquid fuel or chemical products, which belongs to the field of energy and chemical industry. In particular, it relates to a catalyst for producing low-carbon mixed alcohols and liquid hydrocarbons by catalytic conversion of synthesis gas and a preparation method thereof. More specifically, it relates to a Co&Co loaded with carbon as a carrier 2 C catalyst, the active component is Co 2 Nanocomposite particles of C and metallic Co, while SiO 2 as an auxiliary component. Background technique [0002] Low-carbon mixed alcohol (referred to as low-carbon alcohol) refers to the 1 -C 6 A liquid mixture composed of straight-chain primary alcohols, which can be used as alternative fuels, clean gasoline additives or chemicals and chemical raw materials. The research on the direct synthesis of low-carbon alcohols from syngas began in the 1920s. The impact of the two oil crise...

Claims

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Application Information

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IPC IPC(8): B01J23/75B01J31/16B01J21/08B01J21/18C07C27/06
CPCB01J21/08B01J21/18B01J23/75B01J31/1691C07C27/06
Inventor 裴彦鹏郭庆杰胡修德
Owner NINGXIA UNIVERSITY
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