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Copper-based hydrogenation catalyst prepared by flame jet cracking method and its preparation and application

A technology of hydrogenation catalyst and flame injection, which is applied in the direction of metal/metal oxide/metal hydroxide catalyst, physical/chemical process catalyst, heterogeneous catalyst chemical elements, etc. Environmental and human factors have a large impact, hindering the scale-up production of catalysts, etc., to achieve the effect of avoiding sintering aggregation, small environmental and human factors, and obvious modification effect

Active Publication Date: 2020-06-16
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

The catalysts prepared by the above catalyst preparation methods have shown high catalytic performance in the catalytic hydrogenation reaction, but the main problems of these preparation methods are: (1) copper has the characteristics of high temperature and easy sintering aggregation, so the above preparation process The subsequent roasting treatment may cause the copper particles to grow up and reduce the activity; (2) the subsequent roasting treatment may also cause the decomposition of the intermediate species copper phyllosilicate and lose the modulation Cu + / Cu 0 (3) The catalytic performance of the catalyst is greatly affected by its preparation method and preparation conditions, the preparation procedure is complicated, and it is greatly affected by environmental and human factors. The phenomenon of unevenness and non-repeatable performance often occurs in the scale-up preparation process, which is serious Hinders scale-up production of catalysts
The application method of using this technology to prepare copper-based catalysts and use them in hydrogenation reactions has not been reported, and has broad application prospects

Method used

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  • Copper-based hydrogenation catalyst prepared by flame jet cracking method and its preparation and application
  • Copper-based hydrogenation catalyst prepared by flame jet cracking method and its preparation and application
  • Copper-based hydrogenation catalyst prepared by flame jet cracking method and its preparation and application

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0034] 1.89g copper acetate Cu(CH 3 COO) 2 ·H 2 O and 11.2ml of tetraethyl orthosilicate (TEOS) were dissolved in a mixed solvent of 44.4ml of methanol and 44.4ml of 2-ethylhexanoic acid. The solution was placed on a magnetic stirrer and stirred at room temperature until a clear solution was obtained. Use a syringe to pump the prepared solution into the nozzle at a rate of 5 ml / min. Flame combustion gas is a mixture of methane (0.6L / min) and oxygen (1.9L / min), dispersion gas is oxygen (3.5L / min, pressure drop 4.5bar), protective gas is air (5.0L / min) . Catalyst particles from combustion were collected with glass fiber filter paper with the help of a vacuum pump. The prepared catalyst is denoted as FSP-Cu / SiO 2 , the mass fraction of Cu is 20%.

[0035] Reduction conditions before catalyst reaction: under normal pressure, pure H 2 (25ml / min), the temperature is 350°C, and the reduction time is 3h. Reaction conditions: molar ratio H 2 / Methyl acetate (MA) = 80, the te...

Embodiment 2

[0037] 1.89g copper acetate Cu(CH 3 COO) 2 ·H 2 O, 0.80g magnesium acetate Mg(CH 3 COO) 2 4H 2 O and 11.2ml of tetraethyl orthosilicate (TEOS) were dissolved in a mixed solvent of 44.4ml of methanol and 44.4ml of 2-ethylhexanoic acid. The solution was placed on a magnetic stirrer and stirred at room temperature until a clear solution was obtained. Subsequent steps are the same as in Example 1. The prepared catalyst is denoted as FSP-Cu-Mg / SiO 2 , the mass fraction of Cu is 20%, and the mass fraction of MgO is 5%. The reduction conditions and reaction conditions of the catalyst are the same as in Example 1. The test results (see Table 2) show that as the reaction temperature increases, the methyl acetate conversion rate increases gradually, and the ethanol selectivity increases gradually. At 200°C, the conversion rate of methyl acetate was 15.55%, which was 7.5% higher than that of the catalyst without additives (Example 1). It can be seen that in the preparation of c...

Embodiment 3

[0039] 1.89g copper acetate Cu(CH 3 COO) 2 ·H 2 O, 0.41g zinc acetate Zn(CH 3 COO) 2 2H 2 O and 11.2ml tetraethyl orthosilicate (TEOS) were dissolved in a mixed solvent of 44.4ml methanol and 44.4ml 2-ethylhexanoic acid, the mass fraction of Cu was 20%, and the mass fraction of ZnO was 5%. The solution was placed on a magnetic stirrer and stirred at room temperature until a clear solution was obtained. Subsequent steps are the same as in Example 1. The prepared catalyst is denoted as FSP-Cu-Zn / SiO 2 . The reduction conditions and reaction conditions of the catalyst are the same as in Example 1. The test results (see Table 3) show that as the reaction temperature increases, the conversion of methyl acetate increases gradually, and the ethanol selectivity increases gradually. At 200°C, the conversion rate of methyl acetate was 23.80%, which was 15.8% higher than that of the catalyst without additives (Example 1). It can be seen that in the preparation of copper-based c...

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Abstract

The invention provides a copper-based hydrogenation catalyst prepared by flame spray cracking method and its application. The catalyst uses copper as the main active component and can be modified by adding one or more auxiliaries. It is made by flame spray Prepared in one step by lysis method. The invention also relates to the application of the copper-based catalyst prepared by the preparation method in the hydrogenation reaction of carbonyl-containing organic matter. The beneficial effects of the catalyst of the present invention are mainly reflected in: (1) the catalyst in the present invention has small particle size, high metal dispersion, and high low-temperature hydrogenation activity after instantaneous high temperature; (2) the catalyst in the present invention can be quickly prepared through a one-step method, The output per unit time is high, there is no subsequent heat treatment process, and sintering aggregation of copper is avoided; (3) The copper-silicon intermediate species of the catalyst in the present invention is different from the catalyst prepared by the ammonia evaporation method, and has the ability to better condition the valence state of copper.

Description

technical field [0001] The invention relates to a copper-based hydrogenation catalyst and its application, in particular to a copper-based catalyst prepared in one step by a flame jet cracking method, and its application in the hydrogenation reaction of carbonyl-containing organic matter. Background technique [0002] Nanomaterials and nanocatalysts play a vital role in many fields related to the national economy and people's livelihood, such as chemical industry, materials, energy, and environmental protection. There are various preparation methods of nanomaterials, such as traditional impregnation method, precipitation method, hydrothermal synthesis method, ball milling method and chemical reduction method, etc. In addition, sol-gel method, microemulsion synthesis method, citric acid complexation method and supercritical Fluid technology is also a common method for preparing nanocatalysts. However, these preparation methods are complicated to operate and have a long prepa...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/72B01J23/78B01J23/80C07C29/149C07C31/08B01J35/02B01J35/00
CPCC07C29/149B01J23/72B01J23/78B01J23/80B01J2523/00B01J35/393B01J35/394B01J35/40B01J2523/17B01J2523/41B01J2523/22B01J2523/27C07C31/08
Inventor 俞佳枫张哲张继新徐恒泳
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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