One-step method used for synthesis of iron-based molecular sieve catalyst, and applications thereof

A molecular sieve and catalyst technology, applied in the field of chemistry, can solve problems such as disadvantages

Active Publication Date: 2019-07-09
HUAZHONG UNIV OF SCI & TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, there are a series of problems in the preparation of Fe-zeolite molecular sieve catalysts by the traditional ion exchange method: due to the hydration of Fe 3+ The ionic radius is much larger than the pore diameter of molecular sieves (Appl.Catal.B:Environ.180(2016)775–787)
However, there is another problem in the one-pot synthesis of Fe-based aluminosilicate molecular sieves: the synthetic aluminosilicate molecular sieve gel system is generally in an alkaline environment. If Fe salt is directly added to the gel, it will cause Fe salt to form a precipitate. During the ion exchange process in the later stage of molecular sieve, it is difficult to form Fe 3+ Entering the molecular sieve exchange site, most of Fe exists in the form of oxides, which is not conducive to NH 3 -SCR response

Method used

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  • One-step method used for synthesis of iron-based molecular sieve catalyst, and applications thereof
  • One-step method used for synthesis of iron-based molecular sieve catalyst, and applications thereof
  • One-step method used for synthesis of iron-based molecular sieve catalyst, and applications thereof

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Experimental program
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Effect test

Embodiment 1

[0061] Embodiment 1: Synthesis of Fe-ZSM-5 molecular sieve catalyst

[0062] Dissolve 0.9g of sodium hydroxide in 22g of deionized water, add 0.51g of sodium metaaluminate after it is fully dissolved, and stir to fully dissolve to obtain solution A. Dissolve 15g of silica sol in 10g of deionized water, then add 3g of tetrapropylammonium bromide, stir thoroughly to obtain solution B, and slowly add solution B to solution A under stirring. Dissolve 0.33g disodium ethylenediaminetetraacetic acid in 10g deionized water, add 0.27g ferrous sulfate after it is completely dissolved, obtain Fe-complex solution after fully complexing, and prepare Fe-complex The solution was slowly added in batches to the mixed solution of A and B, stirred for 4h and then left to stand for 24h. Then it was loaded into a kettle and crystallized at 170°C for 48h. The obtained product was washed with deionized water, suction filtered, dried at 110°C for 12 hours, and then calcined at 600°C for 6 hours to ...

Embodiment 2

[0063] Embodiment 2: Synthesis of Fe-Beta molecular sieve catalyst

[0064] Dissolve 1.68g of sodium hydroxide in 24g of deionized water, add 0.35g of sodium metaaluminate after it is fully dissolved, and stir to fully dissolve to obtain solution A. Dissolve 3.6g of fumed silica in 10g of deionized water, then add 2.56g of tetrapropylammonium bromide, stir well to obtain solution B, and slowly add solution B into solution A while stirring. Dissolve 0.33g disodium ethylenediaminetetraacetic acid in 10g deionized water, add 0.27g ferrous sulfate after it is completely dissolved, obtain Fe-complex solution after fully complexing, and prepare Fe-complex The solution was slowly added in batches to the mixed solution of A and B, and stirred for 4h. Then it was loaded into a kettle and crystallized at 120°C for 144h. The obtained product was washed with deionized water, filtered with suction, dried at 110°C for 12 hours, and then calcined at 600°C for 6 hours to remove the organic te...

Embodiment 3

[0065] Embodiment 3: Synthesis of Fe-SSZ-13 molecular sieve catalyst

[0066] Dissolve 0.81 g of sodium hydroxide in 25.3 g of deionized water, add 2 g of sodium metaaluminate after it is fully dissolved, and stir to fully dissolve to obtain solution A. Dissolve 20g of silica sol in 10g of deionized water, then add 13.55g of N,N,N-trimethyl-1-adamantyl ammonium hydroxide, stir thoroughly to obtain solution B, and slowly add solution B to A solution. Dissolve 0.66g disodium ethylenediaminetetraacetic acid in 10g deionized water, add 0.56g ferrous sulfate after it is completely dissolved, obtain Fe-complex solution after fully complexing, and prepare Fe-complex The solution was slowly added in batches to the mixed solution of A and B, and stirred for 4h. Then put it in a kettle and crystallize at 150°C for 96h. The obtained product was washed with deionized water, filtered with suction, dried at 110°C for 12 hours, and then calcined at 600°C for 6 hours to remove the organic ...

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Abstract

The invention provides a one-step method used for synthesis of an iron-based molecular sieve catalyst. The one-step method comprises following steps: a Fe-complex solution and an aluminosilicate molecular sieve gel system are prepared respectively; the Fe-complex solution is added into the aluminosilicate molecular sieve gel system slowly, full stirring is carried out, an obtained mixture is allowed to stand for aging, is introduced into a reaction kettle for crystallization, is washed with deionized water, and is subjected to pumping filtration, drying, and roasting so as to obtain a solid iron-based molecular sieve; and then ammonium exchange is carried out so as to obtain the iron-based molecular sieve catalyst. The technology of the one-step method is simple; adoption of a plurality oftimes of ammonium nitrate and iron salt solution ion exchange and calcining is avoided, a defect in the prior art that later stage ion exchange technology is needed for loading of the active component is avoided, the synthesized iron-based molecular sieve catalyst is better in catalytic activity, Fe distribution is more uniform, excellent NH3-SCR catalytic activity is maintained in a wider temperature window, and at the same time, excellent high temperature activity and N2 selectivity are achieved.

Description

technical field [0001] The invention belongs to the field of chemistry, and relates to a preparation method of an iron-based molecular sieve catalyst (Fe-zeolite), and the catalyst prepared by the method is used for the selective catalytic reduction of nitrogen oxides (NH 3 -SCR) process. Background technique [0002] Environmental issues have become a hot issue in the current society, and the harm caused by nitrogen oxides to the environment is becoming more and more significant. As a major air pollutant, nitrogen oxides mainly come from factory exhaust and motor vehicle exhaust. Among them, diesel vehicle exhaust nitrogen oxides (NO x ) pollution has become one of the most prominent problems in my country's air pollution. In mobile source denitrification, selective catalytic reduction of ammonia (NH 3 -SCR) to eliminate nitrogen oxides (NO x ) has become the most potential and widely used denitrification technology due to its advantages of high efficiency and low cost...

Claims

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Application Information

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IPC IPC(8): B01J29/46B01J29/76B01D53/94B01D53/56C01B39/06
CPCB01D53/9413B01D2251/2062B01D2258/012B01J29/46B01J29/76B01J29/7615B01J29/763B01J2229/183C01B39/065C01P2002/72Y02A50/20Y02C20/10Y02T10/12
Inventor 李涛陈真范驰
Owner HUAZHONG UNIV OF SCI & TECH
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