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Catalyst for catalytically removing nitrogen oxides at low temperature and preparation method thereof

A technology for low-temperature catalysis and nitrogen oxides, applied in the field of low-temperature catalytic removal of nitrogen oxides in diesel engine exhaust and its preparation, low-temperature catalytic removal of nitrogen oxides and its preparation, can solve the problems affecting catalyst activity and stability, Problems such as poor catalytic activity and selectivity, low catalytic activity of molecular sieves, etc., to achieve stable and excellent low-temperature SCR performance, low price, and improved stability

Active Publication Date: 2021-06-29
SHANGHAI JIAOTONG UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0004] The main method of synthesizing Fe-ZSM-5 catalyst is solid / liquid ion exchange and impregnation method at present, but there are following problems: the first, the iron content of Fe-ZSM-5 catalyst prepared by ion exchange method is not high at present, generally at 3% Below, and generally two or more times of exchange times are required for repeated roasting to achieve a higher iron content in the Fe-ZSM-5 catalyst, but repeated roasting is likely to cause defects in the crystal skeleton of the Fe-ZSM-5 catalyst, affecting the activity of the catalyst and stability
Second, although the existing impregnation method can make the Fe-ZSM-5 catalyst support a high iron content, most of its active sites exist on the surface of the molecular sieve, and they are clustered together in the form of oxides, resulting in the catalytic activity of the molecular sieve. Not active
However, in this method, due to the adjustment of the pH of the solution, the active metal elements are deposited on the "outer" or "inner" surface of the molecular sieve at specific sites, which will inevitably lead to a large amount of iron in the form of iron oxide, resulting in poor catalytic activity and selectivity.

Method used

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  • Catalyst for catalytically removing nitrogen oxides at low temperature and preparation method thereof
  • Catalyst for catalytically removing nitrogen oxides at low temperature and preparation method thereof
  • Catalyst for catalytically removing nitrogen oxides at low temperature and preparation method thereof

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Embodiment 1

[0049] This embodiment relates to the influence of different solvents on the SCR activity of iron / beta zeolite catalysts when oxalic acid is added as organic matter, and its preparation method includes the following steps:

[0050] 1. Ferric acetate is used as the iron source, oxalic acid is used as the organic compound, and the molar ratio of the iron element in the organic compound to the iron source is 1:1. The comparison uses water or ethanol or a mixture of both as solvent.

[0051] 2. The different sample solutions were evaporated to dryness with stirring at 90°C, and dried in an oven at 110°C for 12 hours.

[0052] 3. Put the powdered solid sample into a corundum crucible with a volume of 200mL, then place the sample-filled crucible in a muffle furnace, raise the temperature to 550°C at a rate of 5°C / min, and keep it warm for 4h. After cooling, take it out and grind it in an agate mortar to obtain the target product. In the prepared catalyst, the mass percent content ...

Embodiment 2

[0057] This embodiment relates to the influence of different solvents on the SCR activity of iron-based MFI molecular sieve catalysts when citric acid is added as organic matter, and its preparation method includes the following steps:

[0058] 1. Ferric acetate is used as the iron source, citric acid is used as the organic compound, and the molar ratio of the iron element in the organic compound to the iron source is 9: 1, and water or methanol or a mixture of the two is used as a solvent for comparison.

[0059] 2. The different sample solutions were evaporated to dryness with stirring at 90°C, and dried in an oven at 110°C for 12 hours.

[0060] 3. Put the powdered solid sample into a corundum crucible with a volume of 200mL, then place the sample-filled crucible in a muffle furnace, raise the temperature to 550°C at a rate of 5°C / min, and keep it warm for 4h. After cooling, take it out and grind it in an agate mortar to obtain the target product. In the prepared catalyst,...

Embodiment 3

[0065] This embodiment relates to the influence of different organic matter additions on the SCR activity of the iron / beta zeolite catalyst, and its preparation method comprises the following steps:

[0066] 1. Using ferric nitrate as the iron source, compared to using a mixture of water and ethanol as the solvent.

[0067] 2. Add oxalic acid or citric acid or urea with 5 times molar ratio of iron to the above solution, stir and disperse, stir and evaporate different sample solutions at 90°C, and dry them in an oven at 110°C for 12h.

[0068] 3. Put the powdered solid sample into a corundum crucible with a volume of 200mL, then place the sample-filled crucible in a muffle furnace, raise the temperature to 550°C at a rate of 5°C / min, and keep it warm for 4h. After cooling, take it out and grind it in an agate mortar to obtain the target product. In the prepared catalyst, the mass percent content of iron was 5%.

[0069] 4. Extruding, crushing and sieving the obtained differen...

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Abstract

The invention provides a catalyst for catalytically removing nitrogen oxides at low temperature and a preparation method thereof. The catalyst is an iron-based molecular sieve with high iron content; the preparation method comprises: stirring and mixing the molecular sieve with an iron salt substance and at least one organic compound under the conditions of deionized water and at least one alcohol mixed solvent, and then drying Dry, calcined. After calcination to remove the organic compounds in the mixture, heat at 350-800°C for 2-6 hours in a reducing atmosphere, and then conduct passivation treatment in an air atmosphere. Compared with iron-containing molecular sieves without mixed solvents, organic compounds, heat treatment under reducing atmosphere and air passivation, this technology significantly increases the active sites of iron on molecular sieves, broadens the active range, and can be used at 125-500°C NO in temperature range x NH 3 ‑SCR conversion efficiency is above 90%.

Description

technical field [0001] The invention belongs to the technical field of environmental catalysis, and in particular relates to a catalyst for the low-temperature catalytic removal of nitrogen oxides and a preparation method thereof, and more particularly relates to a catalyst for the low-temperature catalytic removal of nitrogen oxides in diesel engine tail gas based on molecular sieve improvement and its preparation method. Background technique [0002] With the development of modern industry and the increase in the number of gasoline and diesel locomotives, the emission of nitrogen oxides is still one of the main environmental pollutants. These pollutions not only cause damage to the atmospheric environment (ozone layer hole, acid rain and photochemical smog, etc.), but also seriously endanger human health. Nitrogen-containing reducing agents such as ammonia (NH 3 ) or urea (CO(NH 2 ) 2 ) to remove nitrogen oxides (NO x ) into nitrogen by selective catalytic reduction, ...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J29/46B01J29/72B01J35/02F01N3/10B01J35/00
CPCB01J29/46B01J29/7215F01N3/10B01J2229/18F01N2570/14B01J35/40
Inventor 石琎上官文峰
Owner SHANGHAI JIAOTONG UNIV
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