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Ammonia synthesis catalyst and preparation method thereof

A catalyst, ammonia synthesis technology, applied in the production of bulk chemicals, etc., can solve the problem of low activity, and achieve the effect of improving ammonia synthesis activity and good application prospects

Inactive Publication Date: 2012-12-19
FUZHOU UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Low activity, and there is the influence of chloride ions

Method used

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  • Ammonia synthesis catalyst and preparation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0019] 0.04 mol / L Ce(NO 3 ) 3 ·6H 2 O solution and a certain amount of AgNO 3 Dissolved in a certain amount of deionized water to form A liquid, wherein the amount of silver is 6% of the weight of the ceria carrier in terms of silver simple substance. A certain stoichiometric K 2 RuO 4 (Based on ruthenium simple substance, the weight is 4% of the ceria carrier) dissolved in a certain amount of 2.0 mol / L potassium hydroxide solution to form B solution. Add solution A to solution B dropwise under stirring at room temperature to obtain a black precipitate. Aged at 60°C for 1 h, took it out and let it stand to cool to room temperature, and after high-speed centrifugation, it was washed with deionized water several times to remove potassium nitrate and unreacted potassium hydroxide. Finally, it was dried in an oven at 85 °C for 12 h in H 2 / N 2 Calcined at 500 °C for 1 h in a mixed gas to obtain Ag-Ru / CeO 2 (CP) catalyst. The catalyst is at 10 MPa, 450 ℃, 10000 h -1 At s...

Embodiment 2

[0021] Weigh 12.62 g Ce(NO 3 ) 3 ·6H 2 O was dissolved in 50 ml of deionized water as solution A. Take by weighing potassium ruthenate (the weight in terms of ruthenium is 4% calculation of ceria weight) and press (Ce 4+ +4OH - = Ce(OH) 4 ↓) The precipitant KOH 1.2 times the theoretical value is dissolved in 50 ml deionized water as solution B. Add solution B to solution A dropwise under stirring at room temperature to obtain a black precipitate. Dissolve 0.4720 g of silver nitrate in 100 ml of deionized water as solution C. Disperse the above black precipitate evenly in liquid C again, adjust the pH value to 10 under strong stirring, so that the silver is completely deposited on the catalyst, age at 60 °C for 1 h under slight stirring, take it out and cool it to room temperature, centrifuge, and use After washing with deionized water three times, the precipitate was dried at 85 °C for 12 h, and then calcined in a muffle furnace at 400–500 °C for 2 h. Get 6%Ag-Ru / CeO ...

Embodiment 3

[0023] Weigh 12.62 g Ce(NO 3 ) 3 ·6H 2 O is dissolved in 50 ml deionized water to be liquid A, and potassium ruthenate (the weight in terms of ruthenium is calculated as 4% of the weight of cerium oxide) is weighed and calculated according to (Ce 4+ +4OH - = Ce(OH) 4 ↓) The precipitant KOH which is 1.2 times the theoretical value is dissolved in 50 ml deionized water to form B solution. Add solution A to solution B drop by drop at room temperature under a certain intensity of stirring. Aged for 1 h, taken out and cooled to room temperature, centrifuged, washed with deionized water three times, the precipitate was dried at 95 °C for 12 h, and then calcined in a muffle furnace at 400-500 °C for 2 h. The 0.6 mol / L silver nitrate solution was impregnated in the Ru / CeO 2 catalyst, dried. Get 6%Ag-Ru / CeO 2 Ammonia synthesis catalyst. The catalyst is 10 MPa, 400 ℃, 10000 h -1 At space velocity, the outlet ammonia concentration is 9.4%.

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Abstract

The invention relates to an ammonia synthesis catalyst, in particular to a low-temperature high-activity ammonia synthesis catalyst taking precious metal ruthenium as an active constituent, taking cerium dioxide as a carrier and taking a silver-bearing compound as an auxiliary and a preparation method thereof, wherein the loading of the active constituent ruthenium by weight of the ruthenium is 2-10% of the weight of the carrier cerium dioxide; the loading of the silver auxiliary by weight of the silver is 2-10% of the weight of the carrier cerium dioxide; and co-precipitation, deposition-precipitation and impregnation methods are respectively adopted. The catalyst provided by the invention is mainly used for synthesizing ammonia by utilizing a mixture gas of hydrogen and nitrogen. The strong interaction between the carrier and metal is utilized so as to benefit to reduction of the cerium dioxide; electrons can be transferred to the ruthenium by utilizing the reduced cerium dioxide soas to benefit to decomposition of nitrogen; adsorption of hydrogen can be restrained through the metal strong interaction; and therefore, compared with a conventional ruthenium based ammonia synthesis catalyst taking oxide as the carrier, the catalyst provided by the invention has the characteristics of stable performance and high low-temperature activity.

Description

technical field [0001] The invention belongs to the technical field of fertilizer catalysts, and more specifically relates to an ammonia synthesis catalyst and a preparation method thereof. Background technique [0002] Compared with the traditional molten iron catalyst, the ruthenium-based ammonia synthesis catalyst has the characteristics of low temperature, low pressure and high activity, and is known as the second-generation ammonia synthesis catalyst after the molten iron catalyst. A ruthenium-based ammonia synthesis catalyst is mainly composed of active metal ruthenium, a carrier and an auxiliary agent. Chinese patent CN1270081A discloses an ammonia synthesis catalyst with ruthenium as an active component, activated carbon as a carrier, and alkali metals and alkaline earth metals as auxiliary agents. Carbon-supported ruthenium catalysts with alkali metals, alkaline earth metals, and rare earth metals as additives have the characteristics of low temperature and high act...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/66
CPCY02P20/52
Inventor 林建新张留明倪军王榕林炳裕魏可镁
Owner FUZHOU UNIV