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Supported monatomic copper-based metal oxide catalyst, preparation method and application

A catalyst and metal-based technology, applied in the direction of metal/metal oxide/metal hydroxide catalyst, hydroxyl compound preparation, catalyst activation/preparation, etc., can solve the problems of difficult activation of carbon dioxide, reduced catalyst stability, and low selectivity of methanol products To achieve the effect of inhibiting the production of carbon monoxide and improving the stability of the reaction

Pending Publication Date: 2021-11-26
FUZHOU UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Carbon dioxide hydrogenation to methanol synthesis is an exothermic reaction. According to Le Chatelier's principle, low temperature is more conducive to the formation of methanol, but it is difficult to activate carbon dioxide at low temperature kinetically. Therefore, increasing the temperature will inevitably increase the selectivity of the by-product carbon monoxide
The second aspect is that higher metal loading tends to cause copper to form larger particles, which often cause sintering deactivation under the influence of reaction atmosphere and water, which greatly reduces the stability of the catalyst.
[0009] The above studies show that the Cu-based catalysts obtained by conventional synthesis strategies generally have the disadvantages of high reaction temperature and low methanol product selectivity.

Method used

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  • Supported monatomic copper-based metal oxide catalyst, preparation method and application
  • Supported monatomic copper-based metal oxide catalyst, preparation method and application
  • Supported monatomic copper-based metal oxide catalyst, preparation method and application

Examples

Experimental program
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Effect test

Embodiment 1

[0036] Weigh 0.145g Cu(NO 3 ) 2 ·3H 2 O, 12.622g Zr(NO 3 ) 4 ·5H 2 O was dissolved in 100ml of deionized water to make a clear solution with a total concentration of metal ions of 0.3M, which was designated as solution A. 6.391g anhydrous Na 2 CO 3 Dissolve in 100ml deionized water to make a 0.6M clear solution, which is designated as solution B. Weigh 100ml of deionized water and heat it to 80°C, and record it as solution C. Under the reaction condition of 80°C, solutions A and B were simultaneously added dropwise to solution C at a rate of 0.3ml / min through a peristaltic pump, and then stirred for 0.5h after the precipitation was completed and aged at 80°C for 2h. Subsequently, the precipitate was washed to neutrality by in-situ slow precipitation method. The specific operation was to add the obtained precipitate into 1.5 L of deionized water at 80°C, stir rapidly for 0.5 h, then let it stand and pour off the supernatant. Repeat the above steps until the pH is adjus...

Embodiment 2

[0039] Weigh 0.242g Cu(NO 3 ) 2 ·3H 2 O, 12.450g Zr(NO 3 ) 4 ·5H 2 O was dissolved in 100ml of deionized water to make a clear solution with a total concentration of metal ions of 0.3M, which was designated as solution A. 6.391g anhydrous Na 2 CO 3 Dissolve in 100ml deionized water to make a 0.6M clear solution, which is designated as solution B. Weigh 100ml of deionized water and heat it to 80°C, and record it as solution C. Under the reaction condition of 80°C, solutions A and B were simultaneously added dropwise to solution C at a rate of 0.3ml / min through a peristaltic pump, and then stirred for 0.5h after the precipitation was completed and aged at 80°C for 2h. Subsequently, the precipitate was washed to neutrality by in-situ slow precipitation method. The specific operation was to add the obtained precipitate into 1.5 L of deionized water at 80°C, stir rapidly for 0.5 h, then let it stand and pour off the supernatant. Repeat the above steps until the pH is adjus...

Embodiment 3

[0042] Weigh 0.483g Cu(NO 3 ) 2 ·3H 2 O, 12.020g Zr(NO 3 ) 4 ·5H 2 O was dissolved in 100ml of deionized water to make a clear solution with a total concentration of metal ions of 0.3M, which was designated as solution A. 6.391g anhydrous Na 2 CO 3 Dissolve in 100ml deionized water to make a 0.6M clear solution, which is designated as solution B. Weigh 100ml of deionized water and heat it to 80°C, and record it as solution C. Under the reaction condition of 80°C, solutions A and B were simultaneously added dropwise to solution C at a rate of 0.3ml / min through a peristaltic pump, and then stirred for 0.5h after the precipitation was completed and aged at 80°C for 2h. Subsequently, the precipitate was washed to neutrality by in-situ slow precipitation method. The specific operation was to add the obtained precipitate into 1.5 L of deionized water at 80°C, stir rapidly for 0.5 h, then let it stand and pour off the supernatant. Repeat the above steps until the pH is adjus...

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Abstract

The invention discloses a supported monatomic copper-based metal oxide catalyst, a preparation method thereof and application of the supported monatomic copper-based metal oxide catalyst in preparation of derivatives such as methanol by hydrogenation of carbon dioxide at low temperature. The monatomic copper catalyst is prepared by taking copper nitrate trihydrate, zirconium nitrate pentahydrate and zinc nitrate hexahydrate as raw materials, dropwise adding sodium carbonate into the raw materials at a slow rate, precipitating, aging, slowly washing and filtering in situ, drying and calcining at low temperature. The preparation method is simple and easy to implement, safe and high in repeatability, the active metal copper species in the obtained catalyst exist in a monodisperse state and have strong interaction with the carrier, and the monatomic copper catalyst with the loading capacity as high as 15 wt% can be synthesized by changing the proportion of the input metal. The monatomic catalyst contains unique Cu1-O3 active sites, and can highly selectively reduce carbon dioxide into methanol at a low temperature.

Description

technical field [0001] The invention belongs to the field of metal-loaded catalyst preparation and energy catalysis, and in particular relates to a supported single-atom copper-based metal oxide catalyst, a preparation method thereof, and an application in carbon dioxide hydrogenation to methanol. Background technique [0002] With the rapid development of science and technology and industry, my country is now the world's largest carbon emission country. The excessive exploitation and utilization of fossil energy and the excessive emission of carbon dioxide greenhouse gas make my country face a severe energy and environmental crisis. Therefore, it is particularly important to seek a win-win method to solve this problem. The industrial hydrogenation of carbon dioxide to synthesize high value-added chemicals is a strategy that has the best of both worlds, which can not only effectively reduce carbon dioxide emissions but also alleviate the energy crisis. Among many chemical p...

Claims

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Application Information

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IPC IPC(8): B01J23/80B01J37/03C07C29/154C07C31/04
CPCB01J23/80B01J37/03C07C29/154B01J35/394C07C31/04Y02P20/52
Inventor 谭理赵慧博
Owner FUZHOU UNIV
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