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Catalyst of reaction for removing oxynitrides by methane and preparation method thereof

A nitrogen oxide compound and catalyst technology, which is applied in the field of catalyst for removing nitrogen oxide compound from methane and its preparation field, can solve the problems of narrow activity temperature range, complicated preparation method, low catalyst activity, etc., and achieves good water resistance and sulfur resistance performance, The effect of improving removal efficiency and simple preparation method

Inactive Publication Date: 2009-04-15
TAIYUAN UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

U.S. Patent US5149512 reports that the Co-ZSM-5 catalyst prepared by the ion exchange method has the best activity, but the highest conversion rate of nitrogen oxides is only 34%; another U.S. Patent US5260043 improves Co-ZSM by adding rare earth metals and precious metals, etc. -5 catalyst activity, but the effect is not obvious, and the preparation method is relatively complicated
Chinese patent CN1408477A improves the activity of Co-ZSM-5 catalyst by adding cheap zinc, but the highest conversion rate of nitrogen oxides on the Zn-Co-ZSM-5 catalyst after adding zinc promoter is only 57%
[0003] The disadvantages of the above-mentioned existing catalysts are that the catalyst activity is low, and the active temperature range is narrow, and the stability and water resistance and sulfur resistance are poor.

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0017] 29.1g of tetraethylammonium bromide, 29ml of ammonia water, 3.45g of sodium metaaluminate (41wt.% Al 2 O 3 , 35wt.%Na 2 O) and 1.88g of sodium hydroxide were dissolved in 50ml of water, then 83.5ml of silica sol (29wt.%) was added, and after crystallization at 413K for 200 hours, 2.75g of sodium metaaluminate and 1.2g of sodium hydroxide were added, and in Crystallize at 443K for 24 hours to obtain Na-Beta / Mordenite double microporous molecular sieve; use 0.5M NH for Na-Beta / Mordenite double microporous molecular sieve 4 NO 3 Exchange for 24 hours followed by calcination at 823K for 5 hours to obtain H-Beta / Mordenite double microporous molecular sieves. Put 1g of H-Beta / Mordenite double microporous molecular sieve into 30ml of 0.015mol / L cobalt acetate solution, exchange at 80°C for 24h, dry at 110°C for 12 hours, and finally roast at 550°C for 4 hours to obtain the cobalt content. 2.5% Co-HBeta / Mordenite catalyst. The catalyst was ground and pressed into tablets, ...

Embodiment 2

[0029]The preparation of the carrier H-Beta / Mordenite, the preparation of the Co-HBeta / Mordenite catalyst and the activity evaluation method are the same as in Example 1, except that the concentration of cobalt acetate solution used for ion exchange is 0.01mol / L, and the cobalt content is 1.6%. . The reaction results showed that when the reaction temperatures were 400, 450, 500, 550, 600, and 650°C, the conversion rates of NO were 51.2, 73.3, 91.6, 85.1, 78.5, and 65.3%, respectively.

Embodiment 3

[0031] The preparation of the carrier H-Beta / Mordenite, the preparation of the Co-HBeta / Mordenite catalyst and the activity evaluation method are the same as in Example 1, except that the concentration of cobalt acetate solution used for ion exchange is 0.005mol / L, and the cobalt content is 1.0% . The reaction results showed that when the reaction temperatures were 400, 450, 500, 550, 600, 650°C, the conversion rates of NO were 45.8, 67.9, 86.8, 82.5, 74.4, 63.9%, respectively.

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PUM

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Abstract

The invention provides a catalyst for oxynitride removing reaction by using methane, as well as a preparation method thereof. The catalyst is characterized in that a carrier of the catalyst is an H-Beta / Mordenite double-micropore molecular sieve; an active ingredient is cobalt; the weight percentage of the cobalt is between 0.5 and 10 percent; and the weight percentage of H-Beta / Mordenite is between 90 and 99.5 percent. The preparation method for the catalyst adopts an ion exchange method, which is to put H-Beta / Mordenite double-micropore molecular sieve powder into cobalt acetate solution with the concentration of between 0.005 and 0.03mol / L to react for 24 hours at 90 DEG C, wash, filter, dry and roast the powder to obtain the catalyst. The catalyst can allow the conversion rate of oxynitride to reach over 90 percent, has no inactivation phenomenon after maintaining activity for 72 hours, is wide in the operation interval (between 400 and 650 DEG C) of reaction temperature, and shows good performances of resisting water and sulfur at the same time.

Description

technical field [0001] The invention relates to a catalyst for removing nitrogen oxides and a preparation method thereof, in particular to a catalyst for removing nitrogen oxides from methane under oxygen-enriched conditions and a preparation method thereof. Background technique [0002] Nitrogen oxides cause great harm to the ecological environment and human health, and the removal of nitrogen oxides has attracted great attention from all over the world. Existing NH 3 Selective catalytic reduction of nitrogen oxides has been successfully applied to the removal of nitrogen oxides from stationary sources. But NH as a reducing agent 3 There are problems with storage, transportation, pipeline blockage and corrosion, and expensive operation. Therefore, the use of low-carbon hydrocarbons as reducing agents to eliminate nitrogen oxides is more and more popular. Since methane is abundant, cheap and readily available, and exists in the tail gas of almost every fuel, the selectiv...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/76B01J29/80B01D53/56
Inventor 陈树伟李瑞丰闫晓亮郑家军马静红
Owner TAIYUAN UNIV OF TECH
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