Low-temperature sulfur-tolerant denitration catalyst and preparation method and application thereof

A denitrification catalyst and catalyst technology, applied in the direction of catalyst activation/preparation, chemical instruments and methods, physical/chemical process catalysts, etc., can solve the problems of high preparation cost of low-temperature water resistance and sulfur resistance, high low temperature activity, low water resistance and sulfur resistance, etc. , achieve good thermal stability and mechanical properties, good low-temperature activity and sulfur resistance, improve dispersion and water resistance

Active Publication Date: 2020-12-01
DALIAN MARITIME UNIVERSITY
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Problems solved by technology

Guangzhou University disclosed a modified perovskite catalyst and its preparation method in the Chinese patent CN109317153A (2019-2-12). The molecular formula of the catalyst is La 0.6 Sr 0.4 co 1-x Fe x o 3 , has good sulfur resistance, but its water resistance is not high
In the Chinese patent CN104437079A (2015-3025), Xiangtan University disclosed a perovskite catalyst that can directly decompose NO. The element A is barium, and the element B is manganese and magnesium. The method is carried out in a microwave field and can be used in Direct catalytic decomposition of NO under low temperature and high oxygen content conditions, but its preparation method is expensive
Chinese patent CN102019188A (2011-4-20) discloses a SCR magnetic material catalyst, the active component is magnetic iron oxide, and the carrier is a perovskite-type lanthanum-manganese metal complex. The catalyst has a wide reaction temperature, but it is only suitable for Due to the medium and low temperature NH3-SCR technology, it is not very suitable for the denitrification technology in the low temperature area
Tianjin University discloses the preparation method and application of anti-sulfur perovskite catalyst in Chinese patents CN102000582A (2011-4-6) and CN101845306A (2010-9-29). The A element is lanthanum, and the B element is strontium and cobalt. Citric acid and EDTA are used as complexing agents to adjust the pH to 4-5 to form a sol, and then dry and roast the perovskite sample. It has high low-temperature activity and good sulfur resistance, but its water resistance has not been investigated.
[0006] To sum up, the defects of the existing denitrification catalysts are low water and sulfur resistance while denitrification at low temperature, prone to sulfur poisoning or deactivation of the catalyst after adding water, or high cost of preparation for low temperature water and sulfur resistance

Method used

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  • Low-temperature sulfur-tolerant denitration catalyst and preparation method and application thereof
  • Low-temperature sulfur-tolerant denitration catalyst and preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0034] (1) The carrier is prepared by co-precipitation method, and 6.34g Zr(NO 3 ) 4 ·5H 2 O, 2.75gFe(NO 3 ) 3 9H 2 O and 5.34g of metatitanic acid powder were dissolved in water and mixed evenly, then according to Fe 3+ with Zr 4+ Add 1-2 times of the theoretical amount of precipitant required for complete precipitation of ions, including ammonia water, to form a precipitate. After stirring and aging at 40° C. for 4 h, the product was filtered and washed to form a carrier precursor.

[0035] (2) The perovskite catalyst was prepared by the chemical complexation method, and 43.3g La(NO 3 ) 2 ·6H 2 O, 2.9gNi(NO 3 ) 2 ·6H 2 O, 0.291gCo(NO 3 ) 2 ·6H 2 O and 22.34gMn(NO 3 ) 2 4H 2 O was dissolved in water, and 53.46g of ammonium citrate complexing agent was added to form a uniform mixed solution. Then add the carrier precursor obtained in step (1), mix to form a uniform gel, dry the gel at 100°C for 12 hours, and then bake the gel at 350°C for 4 hours to obtain t...

Embodiment 2

[0039] (1) The carrier is prepared by co-precipitation method, and 3.972g Zr(NO 3 ) 4 ·5H 2 O, 1.725gFe(NO 3 ) 3 9H 2 O and 3.349g metatitanic acid powder were dissolved in water and mixed evenly, then according to Fe 3+ with Zr 4+ Add 1-2 times of the theoretical amount of precipitant required for complete precipitation of ions, including ammonia water, to form a precipitate. After stirring and aging at 70° C. for 4 h, the product was filtered and washed to form a carrier precursor.

[0040] (2) The perovskite catalyst was prepared by the chemical complexation method, and 43.3g La(NO 3 ) 2 ·6H 2 O, 5.82gNi(NO 3 ) 2 ·6H 2 O, 0.873gCo(NO 3 ) 2 ·6H 2 O and 19.327gMn(NO 3 ) 2 4H 2 O was dissolved in water, and 53.46g of ammonium citrate complexing agent was added to form a uniform mixed solution. Then add the carrier precursor obtained in step (1), mix to form a uniform gel, dry the gel at 100°C for 12 hours, and then bake the gel at 350°C for 4 hours to obtain...

Embodiment 3

[0044] (1) The carrier is prepared by co-precipitation method, and 12.38g Zr(NO 3 ) 4 ·5H 2 O, 5.374gFe(NO 3 ) 3 9H 2 O and 10.44g metatitanic acid powder were dissolved in water and mixed evenly, then according to Fe 3+ with Zr 4+ Add 1-2 times of the theoretical amount of precipitant required for complete precipitation of ions, including ammonia water, to form a precipitate. After stirring and aging at 80° C. for 4 h, the product was filtered and washed to form a carrier precursor.

[0045] (2) The perovskite catalyst was prepared by the chemical complexation method, and 43.3g La(NO 3 ) 2 ·6H 2 O, 8.72gNi(NO 3 ) 2 ·6H 2 O, 1.164gCo(NO 3 ) 2 ·6H 2 O and 16.57gMn(NO 3 ) 2 4H 2 O was dissolved in water, and 53.46g of ammonium citrate complexing agent was added to form a uniform mixed solution. Then add the carrier precursor obtained in step (1), mix to form a uniform gel, dry the gel at 100°C for 12 hours, and then bake it at 550°C for 4 hours to obtain the l...

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Abstract

The invention provides a low-temperature sulfur-tolerant denitration catalyst and a preparation method and application thereof. The catalyst consists of an active component, an auxiliary agent and a carrier. The active component has a perovskite structure and is a composite oxide containing La, Ni, Co and Mn elements, the auxiliary agent is oxide of Ce and P, and the carrier is a mixture containing iron oxide, titanium oxide and zirconium oxide. The catalyst is prepared by a method of combining chemical precipitation, chemical complexing and impregnation, and the preparation method is simple,mild in condition and low in cost. The NO conversion rate of the catalyst reaches up to 90% within the temperature range of 200-300 DEG C, and the catalyst has excellent sulfur resistance and water resistance.

Description

technical field [0001] The invention relates to the technical field of harmful gas purification and environmental functional materials, in particular to a low-temperature sulfur-resistant denitrification catalyst and its preparation method and application. Background technique [0002] Due to the massive combustion of fossil fuels, the emission of nitrogen oxides has been increasing year by year. According to the data of "China Environmental Statistical Yearbook 2017", the total emission of nitrogen oxides is 18.51 million tons, which is still high. At the same time, our country is a big energy consumer. For a long time, coal will still be the main energy consumption. Harmful pollutants such as sulfur oxides, nitrogen oxides, and dust particles produced by coal combustion will affect the living environment of human beings and human beings after entering the atmosphere. Serious harm to health. In order to achieve sustainable development, reduce the emission of nitrogen oxide...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/889B01J27/18B01J37/03B01J37/08B01J37/02B01D53/86B01D53/56
CPCB01J23/8892B01J27/1804B01J23/002B01J37/031B01J37/036B01J37/082B01J37/0201B01J37/088B01D53/8628B01J2523/00B01J2523/3706B01J2523/3712B01J2523/47B01J2523/48B01J2523/51B01J2523/72B01J2523/842B01J2523/845B01J2523/847
Inventor 陶平赵颖平孙天军邵秘华余忆玄赵宝刚
Owner DALIAN MARITIME UNIVERSITY
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