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A kind of ruthenium-based ammonia synthesis catalyst with cerium oxide as carrier

A cerium oxide and catalyst technology, applied in the field of ruthenium-based ammonia synthesis catalyst and preparation thereof, can solve problems such as unfavorable ruthenium catalyst ammonia synthesis activity, increase in catalyst particle size, etc., achieve inhibition of sintering growth, promotion of interaction, and good application prospects Effect

Active Publication Date: 2020-06-05
FUZHOU UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, heat treatment in an oxygen-containing atmosphere or a hydrogen-containing atmosphere tends to reduce the ruthenium metal precursor too quickly and increase the catalyst particle size, which is not conducive to the ammonia synthesis activity of the ruthenium catalyst.

Method used

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  • A kind of ruthenium-based ammonia synthesis catalyst with cerium oxide as carrier

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0029] Take 3g of cerium oxide and impregnate an equal volume of 0.015 g / mL nitrosoruthenium nitrate aqueous solution into Ru:CeO 2 The mass ratio of the sample is 0.10:1. After drying, the sample is placed in a tube furnace, and a mixed gas of NO and nitrogen is introduced. In terms of volume percentage, the NO in the mixed gas is 2%, and the nitrogen is 98%. The flow rate of the gas is 30 mL / min. After heat treatment at 250°C for 40 hours, in 5% H 2 and 95% Ar mixed gas at 300° C. for 45 hours to obtain the cerium oxide-supported ruthenium-based ammonia synthesis catalyst.

Embodiment 2

[0031] Take 3g of cerium oxide and impregnate an equal volume of 0.015 g / mL nitrosoruthenium nitrate aqueous solution into Ru:CeO 2 The mass ratio of the sample is 0.60:1. After drying, the sample is placed in a tube furnace, and a mixed gas of NO and argon is introduced. In terms of volume percentage, the mixed gas contains 35% NO and 65% argon. The flow rate is 900 mL / min. After heat treatment at 550°C for 4 hours, in pure H 2 The cerium oxide-supported ruthenium-based ammonia synthesis catalyst was obtained by reducing in air at 500° C. for 5 hours.

Embodiment 3

[0033] Take 3g of cerium oxide and impregnate an equal volume of 0.015 g / mL nitrosoruthenium nitrate aqueous solution into Ru:CeO 2 The mass ratio of the sample is 0.30:1. After drying, the sample is placed in a tube furnace, and a mixed gas of NO and helium is introduced. In terms of volume percentage, the mixed gas contains 25% NO and 75% helium. The flow rate is 300 mL / min. After heat treatment at 450°C for 10 hours, in 25%H 2 and 75% He mixed gas at 400 ° C for 10 hours to obtain the cerium oxide-supported ruthenium-based ammonia synthesis catalyst.

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Abstract

The invention relates to a ruthenium-based ammonia synthesis catalyst using cerium oxide as a carrier. The catalyst is prepared by the following method: conducting thermal treatment on a ruthenium nitrosyl nitrate catalyst supported on cerium oxide in a mixed gas containing NO, and then conducting reduction, so as to obtain the catalyst. The invention has the advantages that in the thermal treatment process, existing NO influences rapid decomposition and reduction of ruthenium nitrosyl nitrate, inhibits sintering growth of ruthenium metal particles, improves dispersing of the ruthenium metal particles, and promotes interaction of the ruthenium metal and the cerium oxide carrier, so that the catalyst of the invention has better ammonia synthesis properties, and under same conditions, the catalyst of the invention has an ammonia synthesis reaction rate substantially higher than a cerium-oxide-supported ruthenium catalyst prepared by a traditionally calcining method, a gas-phase reductionmethod and a liquid-phase reduction method, and has better application prospect.

Description

technical field [0001] The invention relates to a preparation method of a ruthenium-based catalyst for ammonia synthesis using nitrogen and hydrogen in the ammonia synthesis industry in the field of chemical fertilizers, in particular to a ruthenium-based ammonia synthesis catalyst with cerium oxide as a carrier and a preparation method thereof. Background technique [0002] The traditional ammonia synthesis catalyst is a molten iron catalyst, which has disadvantages such as high temperature, high pressure and high energy consumption in the production process, which is not conducive to energy saving and consumption reduction in the ammonia synthesis industry. Ruthenium catalyst is known as the second-generation ammonia synthesis catalyst because of its excellent performance, but so far only the ruthenium catalyst supported by activated carbon has achieved industrial application, but the activated carbon support will generate methane under high temperature and high pressure am...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/63C01C1/04
CPCB01J23/63C01C1/0411Y02P20/52
Inventor 林炳裕吴玉远倪军林建新江莉龙
Owner FUZHOU UNIV
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