A nitrogen-doped porous carbon immobilized noble metal catalyst and its preparation method and application

A nitrogen-doped porous carbon, precious metal catalyst technology, applied in catalyst activation/preparation, chemical instruments and methods, physical/chemical process catalysts, etc., can solve noble metal nanoparticle aggregation, unfriendly post-treatment, low natural abundance, etc. problems, to achieve the effect of easy large-scale production and preparation, excellent catalytic performance, and simple synthesis route

Active Publication Date: 2021-02-02
SHANXI UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, the problems of low natural abundance, high cost, skeleton collapse, and environmentally unfriendly post-processing of these raw materials have become bottlenecks that limit their wide application.
Therefore, it is urgent to find a new and efficient way to prepare nitrogen-doped porous carbon catalytic materials with high specific surface area and developed pore structure to overcome the aggregation of noble metal nanoparticles under relatively harsh reaction conditions in current heterogeneous catalytic systems. / Drain and deactivation issues
[0004] And because noble metal nanoparticles undergo hydrogenation, oxidation, and coupling reactions in water, alcohols, and other highly polar reaction media, the strong interaction between them and solvent molecules will cause the active components to fall off the surface of the carrier. , poisoning or deactivation; therefore, it is the key of the present invention to search for a catalyst with low cost, strong operability and high stability of noble metal nanoparticles that can meet mass production

Method used

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  • A nitrogen-doped porous carbon immobilized noble metal catalyst and its preparation method and application
  • A nitrogen-doped porous carbon immobilized noble metal catalyst and its preparation method and application
  • A nitrogen-doped porous carbon immobilized noble metal catalyst and its preparation method and application

Examples

Experimental program
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Effect test

Embodiment 1

[0036] (1) Weigh 1.0g of 1-butyl-3-methylpyridine ionic liquid and 1.0g of chitosan into a mortar and grind them evenly, mix 6.0g of KCl-ZnCl 2 The double salt (mass ratio of the two is 1:1) was added to the above system, transferred to a ball mill and continued to be ball milled to obtain a viscous solid sample.

[0037] (2) Put the obtained solid sample into a high-temperature quartz boat, raise the temperature to 600°C at a rate of 2°C / min under a nitrogen flow rate of 50 mL / min, and keep it for 1 hour before cooling to room temperature.

[0038] (3) The obtained black powder was added to 0.1mol / L hydrochloric acid solution and treated at room temperature for 1 hour, filtered, washed and dried, then added to the palladium acetate solution and ultrasonically treated at room temperature for 0.5 hours, 1.0mmol / LNaBH 4 The solution was added dropwise into the above system and stirred for 2 hours. After suction filtration, water washing and ethanol rinsing, a nitrogen-doped hi...

Embodiment 2

[0042] (1) Weigh 1.0g of ionic liquid and 2.0g of chitosan and add them into a mortar for grinding and mixing, and mix 8.0g of KCl-ZnCl 2 The double salt (mass ratio of the two) was added to the above system, transferred to a ball mill and continued to be ball milled to obtain a viscous solid sample.

[0043] (2) Put the obtained solid sample into a high-temperature quartz porcelain boat, raise the temperature to 700°C at a rate of 3°C / min under a nitrogen flow rate of 50 mL / min, and keep it for 1 hour before cooling to room temperature.

[0044] (3) The obtained black powder was added to 0.1mol / L hydrochloric acid solution and treated at room temperature for 1 hour, filtered, washed and dried, then added to the palladium acetate solution and ultrasonically treated at room temperature for 0.5 hours, 5.0mmol / LNaBH 4 The solution was added dropwise into the above system and stirred for 2 hours. After suction filtration, water washing and ethanol rinsing, a nitrogen-doped hiera...

Embodiment 3

[0047] (1) Weigh 1.0g of ionic liquid and 3.0g of chitosan into a mortar, grind and mix well, mix 9.0g of KCl-ZnCl 2 The double salt (mass ratio of the two is 1:3) was added to the above system, transferred to a ball mill and continued to be ball milled to obtain a viscous solid sample.

[0048] (2) Put the obtained solid sample into a high-temperature quartz porcelain boat, raise the temperature to 800°C at a heating rate of 5°C / min under the condition of a nitrogen flow rate of 100 mL / min, and keep it for 1 hour before cooling to room temperature.

[0049] (3) The obtained black powder was added to 0.2mol / L hydrochloric acid solution and treated at room temperature for 1 hour, filtered, washed and dried, then added to the palladium acetate solution and ultrasonically treated at room temperature for 0.5 hours, 5.0mmol / LNaBH 4 The solution was added dropwise into the above system and stirred for 2 hours. After suction filtration, water washing and ethanol rinsing, a nitrogen...

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Abstract

The invention discloses a nitrogen-doped porous carbon solid-supported noble metal catalyst and a preparation method and application thereof. The preparation method comprises the following steps: (1)placing a mixture of chitosan, an ionic liquid and a KCl-ZnCl2 compound salt in a tube furnace, heating the temperature of the furnace body to 600-1000 DEG C in an atmosphere of continuous introduction of inert gas, and keeping constant temperature for 1-8 hours so as to obtain a black solid; (2) adding the black solid to a dilute acid solution, performing rapid stirring at room temperature for 1-5 hours, and performing the operation of rapid stirring twice so as to remove the compound salt template; and (3) performing ultrasonic dispersion on the obtained material in a palladium salt solutionfor 0.5-2 hours, adding a NaBH4 solution dropwise and slowly into the reaction system, performing stirring for 2-6 hours, performing water washing on the obtained solid product, and drying the washedproduct so as to obtain the catalyst. The catalyst has abundant defect sites, abundant nitrogen content and a developed pore structure, and exhibits superior catalytic performance for selective hydrogenation reactions of quinoline derivatives under mild conditions of 80 DEG C and 0.1 MPa H2.

Description

technical field [0001] The invention relates to a nitrogen-doped porous carbon immobilized noble metal catalyst and a preparation method and application thereof, belonging to the technical field of catalyst preparation and application. Background technique [0002] Chemoselective hydrogenation of quinolines and their derivatives is a very attractive reaction process, since its hydrogenation products 1,2,3,4-tetrahydroquinolines (py-THQs) are widely used in fine chemicals, pesticides , pharmaceuticals and other bioactive molecules play a very critical role. The hydrogenation process of quinoline derivatives often involves multiple intermediates, and the reaction energy barrier is high, resulting in a slow internal kinetic reaction process, which poses more severe challenges to the production and development of high-performance catalysts. Although noble metal-supported catalysts based on Ru, Rh, Au, Pt, and Pd have shown excellent catalytic performance in the selective hydrog...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J27/24B01J35/08B01J35/10B01J37/00B01J37/16C07D215/06
CPCB01J27/24B01J35/006B01J35/1028B01J35/1057B01J35/1061B01J37/0018B01J37/16C07D215/06
Inventor 张锋伟马春兰张献明
Owner SHANXI UNIV
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