Catalyst for preparing low carbon mixed alcohol through synthesis gas and preparation method thereof

A technology of low-carbon mixed alcohols and catalysts, applied in chemical instruments and methods, preparation of hydroxyl compounds, preparation of organic compounds, etc., can solve the problem of low CO conversion rate, structural stability needs further investigation, catalytic reaction performance and product selectivity No advanced problems, achieve the effect of novel structure, prevent agglomeration, and simple synthesis method

Active Publication Date: 2017-06-13
XIAMEN UNIV
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Chinese patent CN103191741A reports a copper-iron core-shell catalyst and preparation method for synthesizing low-carbon alcohols. The core of the catalyst is Fe 2 o 3 , the shell is CuO, the catalyst can prevent iron sintering, but its CO conversion rate is not high (up to 35%), and the methanol content of the product accounts for more than 35%
Although some progress has been made in the above research, the catalytic performance, especially the product selectivity, is still not high, and the structural stability of catalysts with special structures such as the core-shell structure in the reaction process needs to be further investigated.

Method used

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  • Catalyst for preparing low carbon mixed alcohol through synthesis gas and preparation method thereof

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Experimental program
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Embodiment 1

[0027] Weigh 3.53 g of iron acetylacetonate, 14.25 g of cobalt acetylacetonate, 80 mL of dibenzyl ether, 24 mL of oleic acid and 32 mL of oleylamine, then mix them evenly with magnetic stirring, and heat to 150°C for 120 min in a nitrogen atmosphere. After the reacted solution was cooled to room temperature, 60 mL of ethanol was added to wash and centrifuge, repeated 3 times, and then placed in a constant temperature drying oven at 50° C. and dried for 100 min to obtain FeCo-alloy nanoparticles. The FeCo-alloy nanoparticles were re-dispersed into 150 mL of a polyacrylamide absolute ethanol solution with a mass concentration of 8%, and the ultrasound was continued for 120 minutes. Add 2.42g Cu(NO 3 ) 2 ·3H 2 O, continue to stir for 150 minutes, and finally add 2mol / L of NH dropwise 3 ·H 2 O solution, adjust the pH to 10.0. Then, 14 mL of sodium borohydride aqueous solution with a concentration of 5.0 mol / L was quickly added dropwise to obtain a solid suspension with a core-shell...

Embodiment 2

[0032] Weigh 4.04g Fe(NO 3 ) 3 ·9H 2 O, 7.13g cobalt acetylacetonate, 48mL dibenzyl ether, 14.4mL oleic acid, and 19.2mL oleylamine, then mixed with magnetic stirring, and heated to 200°C in a nitrogen atmosphere to react for 60min. After the reacted solution was cooled to room temperature, 80 mL of ethanol was added to wash and centrifuge, repeated twice, and then placed in a constant temperature drying oven at 60° C. for 100 min to obtain FeCo-alloy nanoparticles. The FeCo-alloy nanoparticles were re-dispersed in 120 mL of polyacrylamide anhydrous ethanol solution with a mass concentration of 5%, and the ultrasound was continued for 120 minutes. Add 1.70g CuCl 2 ·2H 2 O, continue to stir for 120min, and finally add 2mol / L of NH dropwise 3 ·H 2 O solution, adjust the pH to 9.0. Then, 14 mL of sodium borohydride aqueous solution with a concentration of 5.0 mol / L was quickly added dropwise to obtain a solid suspension with a core-shell structure. Add 8.0g carrier Al to the susp...

Embodiment 3

[0035] Weigh 4.04g Fe(NO 3 ) 3 ·9H 2 O, 2.91g Co(NO 3 ) 2 ·6H 2 O, 32mL of dibenzyl ether, 9.6mL of oleic acid and 12.8mL of oleylamine, then mixed with magnetic stirring, and heated to 200°C for 120min in a nitrogen atmosphere. After the reacted solution was cooled to room temperature, 80 mL of ethanol was added to wash and centrifuge, repeated twice, and then placed in a constant temperature drying oven at 60° C. and dried for 120 minutes to obtain FeCo-alloy nanoparticles. The FeCo-alloy nanoparticles were re-dispersed in 80 mL of polyacrylamide absolute ethanol solution with a mass concentration of 4%, and the ultrasound was continued for 120 minutes. Add 2.50g CuSO 4 ·5H 2 O, continue to stir for 120min, and finally add 2mol / L of NH dropwise 3 ·H 2 O solution, adjust the pH to 10.0. Then, 20 mL of sodium borohydride aqueous solution with a concentration of 5.0 mol / L was quickly added dropwise to obtain a solid suspension with a core-shell structure. Add 8.0g carrier ZrO t...

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Abstract

The invention relates to a catalyst for preparing low carbon mixed alcohol through synthesis gas and a preparation method thereof, which relate to low carbon mixed alcohol. The catalyst is a supported FeCo-alloy@Cu core-shell structure catalyst; a core layer of the core-shell structure is FeCo-alloy; a shell layer is Cu; an active phase of the core-shell structure FeCo-alloy@Cu accounts for 10 percent to 50 percent, and the balance is a carrier. The preparation method comprises the steps of mixing ferric salt, cobalt salt, dibenzyl ether, oleic acid and oleylamine; cooling a solution subjected to heating reaction, washing, centrifuging, and drying to obtain FeCo alloy nano particles which are denoted as the FeCo-alloy; re-dispersing the FeCo-alloy into absolute ethyl alcohol containing polyacrylamide for carrying out ultrasonography; adding a copper-bearing compound, adding an NH3.H2O solution to obtain a solution A, then adding a sodium borohydride solution, and obtaining a solid suspension liquid with the core-shell structure; then adding a carrier, stirring, carrying out extraction filtration, washing, and reducing dried solid to obtain the catalyst.

Description

Technical field [0001] The present invention relates to low-carbon mixed alcohols, in particular to a catalyst for preparing low-carbon mixed alcohols from synthesis gas and a preparation method thereof. Background technique [0002] With the increasing scarcity of petroleum resources, it is urgent to actively seek and develop new technologies to replace or partially replace non-renewable petroleum resources. In recent years, the use of renewable biomass, natural gas (shale gas) or coal through synthesis gas (CO+H 2 ) The conversion of platform molecules to low-carbon mixed alcohols and other high-value chemicals has become a research hotspot in the field of energy and chemical engineering, and it is also a very important research direction in the field of C1 chemistry. [0003] At present, the catalysts for preparing low-carbon mixed alcohols from synthesis gas mainly include precious metal catalysts, modified methanol synthesis catalysts, modified Fischer-Tropsch synthesis cataly...

Claims

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Application Information

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IPC IPC(8): B01J23/75C07C29/156C07C31/02
CPCC07C29/156B01J23/75B01J35/396B01J35/393C07C31/02
Inventor 王野何顺康金灿张庆红
Owner XIAMEN UNIV
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