Preparation method and application of porous La1-xCexCoO3 perovskite catalyst

A catalyst and mixed solvent technology, applied in the preparation and application of new materials, can solve the problems of reduced catalyst selectivity and high price, and achieve the effects of good catalytic oxidation activity and stability, low price and good catalytic performance

Inactive Publication Date: 2015-04-29
SOUTH CENTRAL UNIVERSITY FOR NATIONALITIES
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  • Description
  • Claims
  • Application Information

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Problems solved by technology

The former is expensive and needs to be in the nanometer size range to achieve ideal catalytic performance
In addition, in many reactions, this type of catalyst needs to add an additional basic promoter to activate the reaction, which will reduce the selectivity of the catalyst for the reaction
Although the latter does not require additional promoters, the oxygen vacancies that are part of the active sites will be repaired by molecular oxygen during the reaction process, and its catalytic efficiency and sustainable utilization are another new challenge.

Method used

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  • Preparation method and application of porous La1-xCexCoO3 perovskite catalyst
  • Preparation method and application of porous La1-xCexCoO3 perovskite catalyst
  • Preparation method and application of porous La1-xCexCoO3 perovskite catalyst

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Experimental program
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Effect test

Embodiment 1

[0034] A La 1-x Ce x CoO 3 The catalyst is prepared by a sol-gel method, and its specific preparation steps are as follows:

[0035] (1) The lanthanum nitrate and cerium nitrate mixture, 5mmol cobalt nitrate that the total molar number is 5mmol are joined in the mixed solvent that is made up of 3mL ethylene glycol and 2mL methanol, stir and dissolve;

[0036] (2) drying the reaction mixture obtained in step (1) in an oven at 95°C to obtain a gel-like solid;

[0037] (3) After taking out the gelatinous solid obtained in step (2), place it in a muffle furnace for calcining and crystallization to obtain the target product, and take it out to obtain La 1-x Ce x CoO 3 catalyst.

[0038] The process of calcination and crystallization in the muffle furnace is as follows: the temperature is raised from room temperature to 600° C. at a rate of 1° C. / min, kept for 5 hours, and then naturally cooled to room temperature.

[0039] Said x is the mole fraction of cerium nitrate in the...

Embodiment 2

[0049] Four kinds of La that embodiment 1 prepares respectively 1-x Ce x CoO 3 (x=0, 0.05, 0.1, 0.15) the catalytic performance of the catalyst in the catalytic oxygen oxidation of benzyl alcohol to benzaldehyde is tested:

[0050] The experimental process is as follows: Take 20 mL of toluene, 20 μL of benzyl alcohol, 10 μL of dodecane (as an internal standard), 0.05 g of catalyst, mix and stir in a three-necked flask, and pass O 2 (99.99%), the flow rate was 50 mL / min, and the reaction temperature was maintained at 88°C. The product was analyzed by gas chromatography, and the detector was flame ionization detector, separation column HP-5 capillary column, H 2 For the carrier gas. The conversion rate of benzyl alcohol is as attached Figure 6 As shown in A. It can be seen from the figure that the addition of a small amount of Ce improves the activity of the reaction and reaches the maximum when x=0.1, indicating that the incorporation of Ce in the perovskite lattice help...

Embodiment 3

[0052] To illustrate the necessity of the presence of a catalyst for the reaction, we examine the La 0.9 Ce 0.1 CoO 3 Catalyst before and after filtration to the catalytic activity of benzyl alcohol oxidation to benzaldehyde reaction as a function of time, see the attached Figure 6 b. Reaction conditions and experimental process are with embodiment 2. It can be seen that when the catalyst exists, the reaction activity gradually increases with the prolongation of time, and when the catalyst is removed, the reaction activity basically does not change, indicating that the reaction is not a homogeneous reaction, but mainly depends on La 0.9 Ce 0.1 CoO 3 Catalytic ability of the catalyst.

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Abstract

The invention belongs to the technical field of preparation and application of new materials, and in particular discloses a preparation method of a Ce-doped perovskite catalyst La(1-x)CexCoO3 (x is more than or equal to 0 and less than or equal to 0.15) and application of the catalyst in catalyzing oxygen to oxidize benzyl alcohol into benzaldehyde under constant pressure. In the method, mixing liquid of ethylene glycol and methanol is used as a solvent, and corresponding metal nitrate is dissolved, so that the Ce-doped perovskite catalyst is prepared in a sol-gel method. The obtained catalyst has a good macroporous structure and a large specific surface area; the catalyst is high in catalytic performance in reaction of catalyzing liquid phase molecular oxygen oxidized benzyl alcohol into benzaldehyde and has catalytic activity higher than that of a precious metal catalyst and a metal oxide catalyst which are reported under the same condition. According to the method, the preparation process is simple, the cost is low, the environment-friendly effect is achieved and the product performance is high; a realization condition of the catalyst in the reaction is simple, the activity is higher than that of a document report result, and the catalyst can be recycled and has a good application prospect.

Description

technical field [0001] The invention relates to the technical field of preparation and application of new materials, in particular to a macroporous Ce-doped La 1-x Ce x CoO 3 (0≤x≤0.15) preparation method of perovskite catalyst and its application in catalytic oxygen oxidation of benzyl alcohol to benzaldehyde under normal pressure. Background technique [0002] In the field of organic chemistry, the development of low-cost, high-efficiency, and long-lived liquid-phase chemical intermediates through "green" synthetic methods has always been a challenging topic. Especially with the development of today's society and the requirements of resource and environmental protection and sustainable development, this demand is becoming more and more prominent. [0003] Catalytic oxidation technology is a common method for the synthesis of organic intermediates. Oxygen is the most ideal "green" oxidant in this method. Compared with traditional industrial oxidants such as potassium p...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/83C07C47/54C07C45/38
CPCY02P20/584
Inventor 朱君江李海龙钟林赟
Owner SOUTH CENTRAL UNIVERSITY FOR NATIONALITIES
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