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Catalyst for preparing higher olefins through carbon dioxide hydrogenation and preparation method and application thereof

A technology for producing high-carbon olefins and carbon dioxide, which is applied in the chemical industry, can solve the problems of low hydrogenation activity, low catalyst activity, and low carbon atom utilization, and achieve high space-time yield and high selectivity

Active Publication Date: 2020-05-22
FUDAN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

The disadvantage is that the catalyst activity is low, the selectivity of the by-product CO is high, and the C 4+ = Olefin space-time yield is only 5.9 μmol CO2 g Fe –1 the s –1 (Commun. Chem. 2018, 1, 11)
[0005] In view of the shortcomings of low hydrogenation activity and low utilization rate of carbon atoms in the existing catalysts for carbon dioxide hydrogenation to high-carbon olefins, the present invention uses metal-type sawtooth structure single-walled carbon nanotube bundles (SWNTs) as a carrier and potassium as an auxiliary agent. Iron-based high-efficiency carbon dioxide hydrogenation to high-carbon olefins catalyst, which is used to efficiently convert carbon dioxide into high-carbon olefins, and compares the catalytic properties of catalysts supported by multi-walled carbon nanotubes (MWNTs)

Method used

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  • Catalyst for preparing higher olefins through carbon dioxide hydrogenation and preparation method and application thereof
  • Catalyst for preparing higher olefins through carbon dioxide hydrogenation and preparation method and application thereof
  • Catalyst for preparing higher olefins through carbon dioxide hydrogenation and preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0024] Example 1: Preparation and performance evaluation of catalyst FeK3 / SWNTs with single-walled carbon nanotube bundles as carrier, iron as active component and potassium as promoter.

[0025] (1) Take a certain amount of single-walled carbon nanotube bundles (composed of metal-type zigzag-shaped single-walled carbon nanotubes with a diameter of 0.47 nm) and disperse them in 100 ml of deionized water, sonicate for 2.0 h, and then magnetically stir for 1.0 h; Add a certain concentration of iron salt solution dropwise to the above suspension while stirring. Continue to stir for 6.0 h after the dropwise addition, then evaporate to dryness in a 60°C water bath, then place in an oven at 110°C to dry overnight, and finally place in a tube furnace and roast at 350°C for 4 h under the protection of argon, and after cooling down to room temperature Take out the sample and grind it for later use;

[0026]The Fe / SWNTs catalyst prepared above was dispersed in 100 ml of deionized water...

Embodiment 2

[0030] Example 2: Effect of Reaction Pressure on Carbon Dioxide Hydrogenation to Higher Olefins

[0031] Take 0.2 g FeK3 / SWNTs catalyst and confine it in the middle of the fixed-bed reactor with quartz sand; before the activity evaluation, the catalyst was activated with carbon monoxide at 350 °C for 8 h, and then passed through H 2 / CO 2 The mixed gas of = 3 was reacted at 340°C, and the reaction pressure range was 1.0-3.0 MPa. During the reaction process, high temperature and high pressure sampling valves were used to sample at regular intervals, and the product composition was analyzed online by gas chromatography. The reaction results of this example are shown in Table 2. It can be seen that increasing the reaction pressure can effectively increase the conversion rate of raw materials and the selectivity of high-carbon olefins, and the optimal reaction pressure is 2.0 MPa.

Embodiment 3

[0032] Example 3: Effect of Reaction Temperature on Carbon Dioxide Hydrogenation to Higher Olefins

[0033] Take 0.2 g FeK3 / SWNTs catalyst, and use quartz sand to confine it in the middle of the fixed-bed reactor; before activity evaluation, the catalyst was activated with carbon monoxide at 350 °C for 8 h, and then passed through H 2 / CO 2 The mixed gas of = 3 is reacted at 2.0 MPa, and the reaction temperature range is 270-380°C. During the reaction process, high temperature and high pressure sampling valves were used to sample at regular intervals, and the product composition was analyzed online by gas chromatography. The reaction results of this example are shown in Table 3. It can be seen that moderate reaction temperature can effectively improve the selectivity of higher olefins, and the optimal reaction temperature is 340°C.

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Abstract

The invention belongs to the technical field of chemical engineering, and particularly relates to a catalyst for preparing higher olefins through carbon dioxide hydrogenation and a preparation methodand application thereof. The catalyst disclosed by the invention is formed by taking a sawtooth metal type single-walled carbon nanotube bundle as a carrier and loading iron and potassium active components. In the catalyst, the mass of the iron accounts for 8-30% of the total mass of the catalyst, and the mass of the potassium accounts for 0.2-5.0% of the total mass of metal. The catalyst is usedfor a carbon dioxide hydrogenation reaction, the catalyst can directly and efficiently convert carbon dioxide into high-value olefins, the selectivity reaches 62% or above, and higher olefins accountfor 60% or above. The olefin selectivity of the catalyst is higher than that of a multi-walled carbon nanotube supported catalyst, the catalytic activity is high, carbon dioxide can be hydrogenated togenerate higher olefins at the speed which is three times higher than that of an existing catalyst, and the catalyst has good environmental protection significance and industrial application prospects.

Description

technical field [0001] The invention belongs to the technical field of chemical industry, and in particular relates to a catalyst for producing high-carbon olefins by hydrogenation of carbon dioxide, a preparation method and application thereof. Background technique [0002] Catalytic hydrogenation of the greenhouse gas carbon dioxide and hydrogen from renewable energy to produce high-value chemical and chemical products can not only reduce the climate problems caused by excessive carbon dioxide emissions in the atmosphere, but also reduce the current excessive use of fossil resources. rely. [0003] Olefin products have important industrial application value. Low carbon olefins (C 2 –C 4 = ) is often used as a basic chemical chemical raw material, such as ethylene is widely used in the production of thermoplastic polymers or oligomers, it is also a raw material for other important monomers, such as vinyl chloride, vinyl acetate, styrene and ethylene glycol, some of whic...

Claims

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Application Information

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IPC IPC(8): B01J23/78C07C1/12C07C11/02
CPCB01J23/78C07C1/12C07C11/02Y02P20/52
Inventor 乔明华王顺武
Owner FUDAN UNIV
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