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Method for preparing olefin compound based on catalyst obtained by compounding carbon tubes and transition metals

A technology of transition metals and compounds, which is applied in the field of preparing olefin compounds based on carbon tubes and transition metal composite catalysts, can solve the problems of unfriendly environment, complex catalyst preparation process, high cost, etc., achieve improved stability, mild reaction conditions, The effect of super stable performance

Active Publication Date: 2015-04-29
ZHEJIANG UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Subsequently, the D.S.Su research group reported a two-step synthesis of nano-diamond / CNT-SiC carbon-based catalysts, selecting macroporous SiC foam with high thermal conductivity and mechanical stability as a carrier, and wrapping it on the surface of SiC foam by chemical vapor deposition. A layer of carbon tubes, and then use ultrasonic-assisted impregnation to load commercial nanodiamonds on the substrate. Although the prepared catalyst has a high conversion rate, the preparation process of the catalyst is complicated and the cost is high. In addition, the reported The stability is only 20 hours (Chem.Commun.,2014,50,7810-7812)
Another example is the nanodiamond / carbon nitride hybrid material prepared by Z.K.Zhao et al. (J.Mater.Chem.A.2014, 2, 13442-13451) is obtained by mixing melamine and nanodiamond and calcining to different temperatures. Melamine introduces heteroatom N to improve its catalytic performance, but it requires strong oxidative acid explosion treatment in the preparation process of nanodiamond, which is extremely unfriendly to the environment, and its catalytic stability is only reported at 20 hours.

Method used

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  • Method for preparing olefin compound based on catalyst obtained by compounding carbon tubes and transition metals
  • Method for preparing olefin compound based on catalyst obtained by compounding carbon tubes and transition metals

Examples

Experimental program
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Effect test

Embodiment 1

[0056] Physically mix 1g of glucosamine hydrochloride, 20g of melamine and 0.7g of nickel nitrate, and place the evenly mixed solid powder in an inert atmosphere in a crucible for calcination. Calcining at 1200°C for 0.5-1.5h, and cooling to room temperature in an inert atmosphere after the calcination procedure is finished, to obtain a composite catalyst of 20wt%-25wt% nickel / nickel oxide and 75wt%-80wt% carbon tubes. Transmission electron microscope picture as figure 1 shown.

[0057] The obtained 0.08g catalyst is mixed with 6g quartz sand and packed into a quartz tube reactor with an inner diameter of 5mm. The volume fraction of ethylbenzene in argon is 5%, and the mass space velocity of ethylbenzene is 1.0h -1 , the flow rate is 10mL / min, the reaction temperature is 450°C, and the pressure is normal pressure. After the reaction is stable, it is detected by gas chromatography equipped with a capillary column and a hydrogen flame detector. At the reaction temperature, the...

Embodiment 2

[0059] Physically mix 1g of glucosamine hydrochloride, 20g of melamine and 0.7g of nickel nitrate, and place the evenly mixed solid powder in an inert atmosphere in a crucible for calcination. Calcining at 1200°C for 0.5-1.5h, and cooling to room temperature in an inert atmosphere after the calcination procedure is over, to obtain a composite catalyst of 20wt%-25wt% nickel / nickel oxide and 75wt%-80wt% carbon tubes.

[0060] The obtained 0.08g catalyst is mixed with 6g quartz sand and packed into a quartz tube reactor with an inner diameter of 5mm. The volume fraction of ethylbenzene in argon is 1.0%, and the mass space velocity of ethylbenzene is 1.2h -1 , the flow rate is 10mL / min, the reaction temperature is 500°C, and the pressure is normal pressure. After the reaction is stable, it is detected by gas chromatography equipped with a capillary column and a hydrogen flame detector. At the reaction temperature, the conversion rate of ethylbenzene is 10%, the selectivity of styr...

Embodiment 3

[0062] Physically mix 1g of glucosamine hydrochloride, 20g of melamine and 0.7g of nickel nitrate, and place the uniformly mixed solid powder in an inert atmosphere in a crucible for calcination. After calcination for 1 hour, after the calcination procedure is completed, cool down to room temperature in an inert atmosphere to obtain a composite catalyst of 25wt% nickel / nickel oxide and 75wt% carbon tubes.

[0063] The obtained 0.08g catalyst is mixed with 6g quartz sand and packed into a quartz tube reactor with an inner diameter of 5mm. The volume fraction of ethylbenzene in argon is 1.0%-5.0%, and the flow rate is 10mL / min. The mass space velocity is 1.8h -1 , the reaction temperature is 550°C, and the pressure is normal pressure. After the reaction is stable, it is detected by a gas chromatograph equipped with a capillary column and a hydrogen flame detector. At this reaction temperature, the conversion rate of ethylbenzene is 10-20%, the selectivity of styrene is 97-98%, ...

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Abstract

The invention discloses a method for preparing an olefin compound based on a catalyst obtained by compounding carbon tubes and transition metals. The method comprises the following steps: preheating and vaporizing an alkane compound, mixing the compound with carrier gas, and carrying out a dehydrogenation reaction in a reactor under the action of a catalyst; and collecting the olefin compound after condensation, wherein the catalyst contains 5-30wt% of transition metals / transition metal oxides and 70-95wt% of carbon tubes. The method is used for preparing aliphatic olefin compounds and aromatic olefin compounds, the catalyst compounded based on the carbon tubes and transition metal elements / transition metal oxides is stable to water, air and heat, the catalytic activity is invariable after the continuous experiment of over 150 hours, continuous operation can be realized, activation is not needed, and the catalyst is economic and convenient. According to the method disclosed by the invention, when the catalyst is applied to ethylbenzene gaseous phase direct dehydrogenation so as to prepare styrene, the conversion rate of the alkane compound is not less than10 percent, and the selectivity of the olefin compound can be more than or equal to 97 percent.

Description

technical field [0001] The invention relates to the field of organic synthesis, in particular to a method for preparing olefin compounds based on a catalyst compounded by carbon tubes and transition metals. Background technique [0002] Olefin compounds are important chemical raw materials, which are divided into aliphatic olefin compounds and aromatic olefin compounds. Propylene / isobutylene mainly comes from the co-production or by-product of steam cracking and fluid catalytic cracking in refineries, and can be widely used in the synthesis of polymers, gasoline additives, rubber and various chemical intermediates. With the increasing demand for low-carbon olefins, the traditional production process is difficult to meet market demand. The development of the process of producing low-carbon alkenes from low-carbon alkanes is of great significance for making full use of low-carbon alkanes to open up new sources of alkenes. [0003] The catalytic reaction of dehydrogenation of...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/755B01J23/75B01J23/745C07C5/333C07C15/46C07C11/08C07C11/06
CPCY02P20/52
Inventor 王勇王静魏中哲李浩然王世萍韩传龙
Owner ZHEJIANG UNIV
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