Ethanol gas phase oxidation acetaldehyde preparation catalyst and preparation and application methods thereof

A gas-phase oxidation and catalyst technology, which is used in the preparation of organic compounds, metal/metal oxide/metal hydroxide catalysts, physical/chemical process catalysts, etc., and can solve the problems of high reaction temperature, low catalytic activity, and complicated preparation. , to achieve the effect of simple preparation process, strong controllability and excellent stability

Active Publication Date: 2019-04-05
HUAZHONG UNIV OF SCI & TECH
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  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0005] Aiming at the above defects or improvement needs of the prior art, the present invention provides a copper-containing oxide-supported nano-gold catalyst for the gas-phase oxidation of ethanol to acetaldehyde, the purpose of which is to introduce non-chromium variable valence metal B into the copper-containing oxide Carrier, modulating the redox characteristics of the carrier, forming a synergistic effect between the three active centers of Au-Cu-B, promoting the activation of molecular oxygen and ethanol at low temperatures, inhibiting the deep oxidation of acetaldehyde, and thus improving the catalyst as a whole High low temperature catalytic activity and acetaldehyde selectivity, thereby solving the technical problems of existing ethanol gas phase selective oxidation catalysts containing poisonous metals, complicated preparation, high reaction temperature, low catalytic activity, poor selectivity, and poor stability

Method used

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  • Ethanol gas phase oxidation acetaldehyde preparation catalyst and preparation and application methods thereof
  • Ethanol gas phase oxidation acetaldehyde preparation catalyst and preparation and application methods thereof
  • Ethanol gas phase oxidation acetaldehyde preparation catalyst and preparation and application methods thereof

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preparation example Construction

[0039] The preparation method of above-mentioned catalyst comprises the steps:

[0040] (1) according to the metered molar ratio of A, B and Cu, the metal nitrate of A, B and Cu is dissolved, and the valence state of metal in the metal nitrate here can be the highest valence, also can be the low valence state, to the metal that obtains After adding citric acid and ethylene glycol to the nitrate solution, ultrasonically treat it for 0.5-1 h to obtain a uniform mixed solution a; the total metal concentration of the metal nitrate solution is 2-5 mol / L, and the total molar number of citric acid and the metal is The ratio is 0.1~0.3:1; the volume ratio of ethylene glycol to the metal nitrate solution is 0.05~0.2:1

[0041] (2) Heat the solution a obtained in step (1) in a sand bath at 130-200°C until spontaneous combustion, and the obtained fluffy solid b is roasted in an oxygen-containing atmosphere at 600-1000°C for 3-10 hours to obtain carrier A x B y Cu z o n ;

[0042] (3...

Embodiment 1

[0049] Au / Al for the Production of Acetaldehyde by Gas-Phase Oxidation of Ethanol 1 Cu 1 Fe 1 o n preparation of

[0050] Weigh 7.51g of aluminum nitrate, 4.84g of copper nitrate and 8.08g of ferric nitrate and dissolve them in 25mL of deionized water, then add 3.0g of citric acid and 2mL of ethylene glycol, mix and stir and sonicate for 0.5h, and put the mixed solution at 170°C Heating in a sand bath until spontaneous combustion, grinding the obtained fluffy solid and roasting in a muffle furnace at 900°C for 6 hours, the Al 1 Cu 1 Fe 1 o n carrier. Take out 1.0g carrier and place it in a 50mL round bottom flask, add 30mL deionized water and 0.20g urea, place the flask in a 100°C oil bath and stir for 10min, add 5mL of 10mM HAuCl dropwise 4 Aqueous solution, reflux reaction for 4 hours, after cooling, suction filtration, washing, drying, and calcination in a muffle furnace at 300°C for 4 hours, Au / Al with Au loading of ~1% can be obtained 1 Cu 1 Fe 1 o n catalyst....

Embodiment 2

[0052] Au / Zn for Ethanol Vapor Phase Oxidation to Acetaldehyde 3 Cu 1 Fe 8 o n preparation of

[0053] Weigh 4.46g of zinc nitrate, 1.21g of copper nitrate and 16.16g of ferric nitrate and dissolve them in 25mL of deionized water, then add 3.1g of citric acid and 2mL of ethylene glycol, mix and stir and sonicate for 0.5h, and put the mixed solution at 180°C Heating in a sand bath until spontaneous combustion, grinding the obtained fluffy solid and roasting in a muffle furnace at 800°C for 7 hours, the Zn 3 Cu 1 Fe 8 o n carrier. Take out 1.0g of the carrier and place it in a 50mL round bottom flask, add 30mL of deionized water and 0.20g of urea, place the flask in a 100°C oil bath and stir for 10min, then add 5mL of 10mM HAuCl dropwise 4 Aqueous solution, reflux reaction for 4 hours, after cooling, suction filtration, washing, drying, and roasting in a muffle furnace at 350°C for 3 hours, Au / Zn with Au loading of ~1% can be obtained 3 Cu 1 Fe 8 o n catalyst.

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Abstract

The invention belongs to the field of catalysts and particularly relates to an ethanol gas phase oxidation acetaldehyde preparation copper oxide-supported nanogold catalyst and preparation and application methods thereof. The ethanol gas phase oxidation acetaldehyde preparation copper oxide-supported nanogold catalyst is composed of Au / AxByCuzOn, wherein A is a valent non-changeable metal ion, andB is a valent changeable metal ion; a carrier is efficiently synthesized through a simple low-temperature combustion-roasting method, and the surface acidity and the oxidation-reduction characteristics of the carrier can be adjusted by adjusting the variety and composition of metal elements to further enhance the synergic catalytic effects between nanogold and the carrier and accordingly to achieve stable and efficient ethanol gas phase selective oxidation acetaldehyde preparation. The ethanol gas phase oxidation acetaldehyde preparation copper oxide-supported nanogold catalyst has the advantages of being simple in preparation process, free from toxic and hazardous metals, high in low-temperature catalytic activity and acetaldehyde selectivity and the like and can maintain performance stability for a long time, avoid obvious carbon deposition and sintering and have a potential industrial application prospect.

Description

technical field [0001] The invention belongs to the field of catalysts, and more specifically relates to a copper-containing oxide-loaded nano-gold catalyst for producing acetaldehyde by gas-phase oxidation of ethanol, a preparation method and application thereof. Background technique [0002] With the rapid development of biomass fermentation ethanol technology, the annual production of bioethanol has exceeded 100 billion liters and is increasing year by year, and its price has been lower than that of petrochemical products such as ethylene and gasoline. In addition to being used as a clean fuel to partially replace gasoline, the most promising use of bioethanol is to replace fossil raw materials in the production of bulk chemicals. Compared with the traditional high-cost and high-pollution ethylene-wacker oxidation to acetaldehyde technology, the selective oxidation of ethanol to acetaldehyde is more in line with the requirements of green and sustainable chemical developme...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/89C07C45/38C07C47/07
CPCB01J23/002B01J23/8926B01J23/894B01J23/8946B01J23/8953B01J23/8986B01J2523/00C07C45/38B01J2523/19B01J2523/842B01J2523/17B01J2523/31B01J2523/27B01J2523/22B01J2523/3706B01J2523/72B01J2523/847
Inventor 刘鹏胡文佳王杰
Owner HUAZHONG UNIV OF SCI & TECH
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