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Preparation method of manganese cerium catalyst with high catalytic activity in methane combustion and product

A methane catalytic combustion and catalyst technology, applied in physical/chemical process catalysts, chemical instruments and methods, metal/metal oxide/metal hydroxide catalysts, etc., can solve the problems of high price, low synthesis activity, sintering deactivation, etc. problem, to achieve the effect of low hydrothermal temperature requirement, simple preparation process and large cost advantage

Inactive Publication Date: 2019-05-03
HUAZHONG UNIV OF SCI & TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Noble metal catalysts have good catalytic performance for methane catalysis, but they have the following disadvantages: a. expensive; b. poor thermal stability (<700 ° C), easy to sinter deactivation; c. poor sulfur resistance; d. noble metals in The earth's reserves are limited; the above four points have largely inhibited the widespread application of noble metal catalysts in the catalytic combustion of methane
At the same time, due to the low synthesis activity and poor thermal stability of the one-step synthesis method, it can only be applied to the fields of sewage treatment, VOCs catalytic combustion, etc., and is not suitable for the field of low-concentration methane catalytic combustion (higher than 400 ° C)

Method used

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  • Preparation method of manganese cerium catalyst with high catalytic activity in methane combustion and product
  • Preparation method of manganese cerium catalyst with high catalytic activity in methane combustion and product
  • Preparation method of manganese cerium catalyst with high catalytic activity in methane combustion and product

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0027] Embodiment 1 Two-step synthesis prepares manganese cerium catalyst (Mn / Ce=9 / 1, Mn 2+ / MnO 4 - =1.5)

[0028] Weigh 0.506g Mn(NO 3 ) 2 50wt%H 2 O was dissolved in 100ml deionized water to form solution A; weigh 0.149g KMnO 4 Solid, add it to 100ml deionized water, stir to dissolve and heat to 60°C to form solution B; add A to B dropwise at a certain rate, and stir, use 0.2M KOH solution to stabilize the pH in the range of 4.5±0.1 within; then the resulting mixed solution was heated to 100° C., aged for 0.5 h, filtered, and washed 3-4 times with deionized water and ethanol. Dissolve the precipitate in 140ml deionized water, add 0.144g (NH 4 ) 2 Ce(NO 3 ) 6 , stirred and transferred to a hydrothermal kettle, reacted at 100°C for 4h, filtered, washed with deionized water and ethanol for 3-4 times, and dried at 105°C for 12h. In the muffle furnace, the heating rate was raised to 500°C at a rate of 2°C / min, and the roasting treatment was carried out for 6 hours to...

Embodiment 2

[0029] Embodiment 2 Two-step synthesis prepares manganese cerium catalyst (Mn / Ce=9 / 1, Mn 2+ / MnO 4 - =1.5)

[0030] Weigh 0.326g MnSO 4 4H 2 O was dissolved in 100ml deionized water to form solution A; weigh 0.149g KMnO 4 Solid, add it into 100ml deionized water, stir to dissolve and heat to 100°C to form solution B; add A to B dropwise at a certain rate, and stir, use 0.4M KHCO 3 The pH of the solution is stabilized within the range of 4.5±0.2; then the obtained mixed solution is heated to 70° C., aged for 1 hour, filtered, and washed 3-4 times with deionized water and ethanol. Dissolve the precipitate in 140ml deionized water, add 0.090g Ce(SO 4 ) 2, stirred and transferred to a hydrothermal kettle, reacted at 100°C for 4h, filtered, washed with deionized water and ethanol for 3-4 times, and dried at 70°C for 12h. In the muffle furnace, the heating rate was raised to 500°C at a rate of 2°C / min, and the roasting treatment was carried out for 6 hours to obtain y mn 8...

Embodiment 3

[0031] Embodiment 3 Two-step synthesis prepares manganese cerium catalyst (Mn / Ce=9 / 1, Mn 2+ / MnO 4 - =1.4)

[0032] Weigh 0.172g MnCl 2 Dissolve in 100ml deionized water to form solution A; weigh 0.149g KMnO 4 Solid, add it into 100ml deionized water, stir to dissolve and heat to 60°C to form solution B; add A to B dropwise at a certain rate, and stir, use 0.2M KCO 3 The pH of the solution is stabilized within the range of 4.5±0.3; then the obtained mixed solution is heated to 60° C., aged for 1 hour, filtered, and washed 3-4 times with deionized water and ethanol. Dissolve the precipitate in 140ml deionized water, add 0.144g (NH 4 ) 2 Ce(NO 3 ) 6 , stirred and transferred to a hydrothermal kettle, reacted at 100°C for 4h, filtered, washed with deionized water and ethanol for 3-4 times, and dried at 110°C for 12h. In the muffle furnace, the heating rate was raised to 500°C at a rate of 2°C / min, and the roasting treatment was carried out for 6 hours to obtain y mn 8 ...

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Abstract

The invention discloses a preparation method of a Mn-Ce methane combustion catalyst. The method comprises the following steps: (1) mixing a manganese-based salt Mn<2+> aqueous solution and a potassiumpermanganate (KMnO4) solution, adding an alkali solution and keeping pH of the mixed solution acidic; (2) performing aging treatment on the mixed solution, and performing filtering to obtain a MnOx solid; (3) mixing the MnOx solid and a cerium salt Ce<4+> aqueous solution, performing a hydrothermal reaction, and performing filtering to obtain a MnCeOx solid; and (4) drying the MnCeOx solid, and performing calcination to obtain the Mn-Ce catalyst containing KyMn8O16. The method provided by the invention can obtain the catalyst with better catalytic activity in methane combustion, and the catalyst has stronger thermal stability and sulfur resistance; and compared with other current preparation methods of the Mn-Ce catalyst, the preparation method provided by the invention has a simple preparation process, shorter total time in the preparation process, a high methane conversion rate of the catalyst, and better industrial application value.

Description

technical field [0001] The invention relates to a catalyst and a preparation method thereof, which are suitable for low-concentration methane combustion and low-hydrocarbon waste gas treatment. Background technique [0002] With the rapid development of economy and society, energy consumption is gradually increasing, and coal mines and oil resources are increasingly depleted. Natural gas with methane as the main component is gradually replacing coal mines and oil in the energy structure. At present, the utilization of methane as energy is mainly in the form of high-temperature combustion, which requires at least one of the following two points: a. The concentration of methane is higher than 5vol%; b. It has a stable high temperature (greater than 650°C) zone. This is mainly because methane's highly symmetrical structure makes it the most stable hydrocarbon. Thermal NO at high temperature x It will be produced in large quantities, which is inconsistent with the current incr...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/889F23G7/07
Inventor 方庆艳仲柳余胜辉余志强张成陈刚
Owner HUAZHONG UNIV OF SCI & TECH