CN116139913A - Catalyst for purifying tail gas of explosion-proof diesel engine and preparation method thereof - Google Patents
Catalyst for purifying tail gas of explosion-proof diesel engine and preparation method thereof Download PDFInfo
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- CN116139913A CN116139913A CN202310090264.XA CN202310090264A CN116139913A CN 116139913 A CN116139913 A CN 116139913A CN 202310090264 A CN202310090264 A CN 202310090264A CN 116139913 A CN116139913 A CN 116139913A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/08—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y
- B01J29/10—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y containing iron group metals, noble metals or copper
- B01J29/14—Iron group metals or copper
- B01J29/146—Y-type faujasite
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2258/00—Sources of waste gases
- B01D2258/01—Engine exhaust gases
- B01D2258/012—Diesel engines and lean burn gasoline engines
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
- B01J2229/10—After treatment, characterised by the effect to be obtained
- B01J2229/18—After treatment, characterised by the effect to be obtained to introduce other elements into or onto the molecular sieve itself
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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Abstract
The invention discloses a catalyst for purifying tail gas of an explosion-proof diesel engine and a preparation method thereof, the catalyst comprises 2 steps of preparation of a modified carrier and preparation of the catalyst, the catalyst uses a Y-type molecular sieve as a basic carrier, alumina and cerium oxide are attached to the surface of the Y-type molecular sieve carrier, and the dispersion of active components can be promoted by modifying the Y-type molecular sieve carrier, so that the reducibility and the adsorption capacity of the catalyst are improved, and meanwhile, the active components in the catalyst are a compound of copper oxide, zirconium oxide, silicon dioxide and expanded graphite, wherein the zirconium oxide has strong ion conductivity and is used as an oxygen ion conductor, the transfer capacity of charges is enhanced, more oxygen vacancies are generated, and the activity of the catalyst is enhanced; the expanded graphite has developed pore structure and good adsorption performance, and can adsorb SO generated in the practical application process 2 And steam, the sulfur resistance and the water resistance of the catalyst are improved.
Description
Technical Field
The invention relates to the technical field of catalyst preparation, in particular to a catalyst for purifying tail gas of an explosion-proof diesel engine and a preparation method thereof.
Background
The problems of multiple transportation links, low efficiency, poor safety and the like exist in the traditional transportation mode, and in recent years, the problems are effectively solved by the rising of the trackless rubber-tyred vehicle of the mining explosion-proof diesel engine. The mining trackless rubber-tyred vehicle has short transportation time, large carrying capacity, strong adaptability and high safety, can effectively improve transportation efficiency, is more and more widely applied to coal mine safety production, but as the service life of the mining trackless rubber-tyred vehicle increases, harmful substances (such as NOx, CO, HC, PM and the like) in waste gas discharged by an explosion-proof diesel engine also increase, wherein gases such as CO and CH are not only toxic and harmful, but also are easy to accumulate to cause underground CO sensor alarm, thereby causing mine monitoring and monitoring system alarm and affecting mine safety production.
According to the generation principle of harmful substances in the tail gas of the explosion-proof diesel engine, the most commonly used principle of the tail gas purifying device of the explosion-proof diesel engine at the present stage is to perform catalytic oxidation on the harmful gases in the discharged tail gas to convert the harmful gases into nontoxic and harmless gases, and when the concentration of particulates, HC and CO is reduced by the catalytic oxidizer, SO can be possibly caused due to the strong catalytic oxidation performance of the catalytic oxidizer 2 And the amount of sulfur in the fuel oil converted into sulfate is greatly increased, and the sulfate covers the surface of the catalyst to gradually reduce the activity of the catalyst and finally completely fail, so that the improvement of the low-temperature sulfur poisoning resistance of the catalyst in the use process is a key of the practical application of the catalyst.
Disclosure of Invention
Aiming at the defects of the prior art, the invention aims to provide a catalyst for purifying tail gas of an explosion-proof diesel engine and a preparation method thereof.
In order to achieve the above purpose, the present invention adopts the following technical scheme:
the preparation method of the catalyst for purifying the tail gas of the explosion-proof diesel engine comprises the following steps:
(1) Preparation of modified carrier: placing the Y-type molecular sieve carrier into a mixed solution of aluminum nitrate and cerium nitrate, adding polyethylene glycol, stirring and mixing uniformly, dripping ammonia water to adjust the pH value of the solution to 9-10, placing the solution into a crystallization kettle for reaction, and centrifuging, washing, drying, grinding and roasting after the reaction is completed to obtain a modified carrier;
(2) Preparation of the catalyst: immersing the modified carrier in aqueous slurry containing copper nitrate, zirconium nitrate, expanded graphite and silica sol, carrying out ultrasonic immersion for 1-2h, then blowing with compressed air, drying and roasting to obtain the catalyst.
Preferably, in the step (1), the mass ratio of the Y-type molecular sieve carrier to the mixed solution to the polyethylene glycol is 10-20:100-150:3-6.
Preferably, in the step (1), the mass fraction of the aluminum nitrate is 12-14%, and the mass fraction of the cerium nitrate is 21-22%.
Preferably, in the step (1), the reaction temperature is 150-180 ℃ and the reaction time is 24-36h.
Preferably, in the step (2), the mass ratio of the modified carrier to the aqueous slurry is 1:4-8.
Preferably, in the step (2), the mass fraction of the copper nitrate in the aqueous slurry is 10-15%, the mass fraction of the zirconium nitrate is 4-8%, the mass fraction of the expanded graphite is 20-30%, and the mass fraction of the silica sol is 12-18%.
Preferably, siO in the silica sol 2 The content of (C) is 25-30wt%.
Preferably, in the step (2), the roasting temperature is 500-550 ℃ and the roasting time is 2-4h.
The invention provides the catalyst prepared by the preparation method.
The invention also provides application of the catalyst in purifying tail gas of an explosion-proof diesel engine.
Compared with the prior art, the invention has the following beneficial effects:
(1) According to the invention, the Y-type molecular sieve is used as a basic carrier, alumina and cerium oxide are attached to the surface of the Y-type molecular sieve carrier, and the dispersion of active components can be promoted by modifying the Y-type molecular sieve carrier, so that the reducibility and the adsorption capacity of the catalyst are improved.
(2) The active components in the catalyst prepared by the invention are a compound of copper oxide, zirconium oxide, silicon dioxide and expanded graphite, wherein the zirconium oxide has strong ion conductivity, is used as an oxygen ion conductor, enhances the charge transfer capability, generates more oxygen vacancies and enhances the activity of the catalyst; the expanded graphite has developed pore structure and good adsorption performance, and can adsorb SO generated in the practical application process 2 And steam, effectively avoidSO 2 And the influence of water vapor on the active site of the catalyst core, so that the sulfur resistance and water resistance of the catalyst are improved.
Detailed Description
The present invention will be described in further detail with reference to the following preferred examples, but the present invention is not limited to the following examples.
Unless otherwise specified, the chemical reagents involved in the present invention are all commercially available.
The Y-type molecular sieves used in the present invention were purchased from Shandong polymer chemistry Co., ltd., CAS number: 12173-28-3;
polyethylene glycol is PEG400, purchased from Henan Tongshida Ind Co., ltd;
expanded graphite was purchased from Qingdao Meiterui graphite Co., ltd. And had a particle size of 0.15mm.
Example 1
The preparation method of the catalyst for purifying the tail gas of the explosion-proof diesel engine comprises the following steps:
(1) Preparation of modified carrier: placing 10g Y type molecular sieve carrier in 100g of mixed solution (the mass fraction of aluminum nitrate is 12% and the mass fraction of cerium nitrate is 21%), adding 3g of polyethylene glycol 400, stirring and mixing uniformly, dripping 1mol/L ammonia water to adjust the pH of the solution to 9, placing in a crystallization kettle, reacting for 24 hours at 150 ℃, centrifuging, washing, drying, grinding after the reaction is completed, heating to 500 ℃ in a muffle furnace at a speed of 3 ℃/min, and roasting for 2 hours to obtain the modified carrier;
(2) Preparation of the catalyst: 10g of the modified support was immersed in 40g of an aqueous slurry in which the mass fraction of copper nitrate was 10%, the mass fraction of zirconium nitrate was 8%, the mass fraction of expanded graphite was 20% and silica Sol (SiO) 2 The mass fraction of the catalyst is 12 percent, the catalyst is immersed for 1h by ultrasonic, then the catalyst is purged by compressed air, dried at 100 ℃, and then baked for 2h after being heated to 500 ℃ in a muffle furnace at a speed of 3 ℃/min.
Example 2
The preparation method of the catalyst for purifying the tail gas of the explosion-proof diesel engine comprises the following steps:
(1) Preparation of modified carrier: placing a 20g Y type molecular sieve carrier in 150g of mixed solution (the mass fraction of aluminum nitrate is 14 percent, the mass fraction of cerium nitrate is 22 percent), adding 6g of polyethylene glycol 400, stirring and mixing uniformly, dripping 1mol/L ammonia water to adjust the pH value of the solution to 9, placing the solution in a crystallization kettle, reacting for 36h at 180 ℃, centrifuging, washing, drying and grinding after the reaction is finished, heating to 500 ℃ at a speed of 3 ℃/min in a muffle furnace, and roasting for 2h to obtain a modified carrier;
(2) Preparation of the catalyst: 10g of the modified support was immersed in 50g of an aqueous slurry in which the mass fraction of copper nitrate was 15%, the mass fraction of zirconium nitrate was 6%, the mass fraction of expanded graphite was 30% and silica Sol (SiO) 2 The mass fraction of the catalyst is 18 percent, the catalyst is immersed for 1h by ultrasonic, then the catalyst is purged by compressed air, dried at 100 ℃, and then baked for 2h after being heated to 550 ℃ in a muffle furnace at a speed of 3 ℃/min.
Example 3
The preparation method of the catalyst for purifying the tail gas of the explosion-proof diesel engine comprises the following steps:
(1) Preparation of modified carrier: placing a 16g Y type molecular sieve carrier in 120g of mixed solution (the mass fraction of aluminum nitrate is 13% and the mass fraction of cerium nitrate is 21%), adding 4g of polyethylene glycol 400, stirring and mixing uniformly, dripping 1mol/L ammonia water to adjust the pH of the solution to 9, placing the solution in a crystallization kettle, reacting for 24 hours at 160 ℃, centrifuging, washing, drying and grinding after the reaction is finished, heating to 500 ℃ in a muffle furnace at a speed of 3 ℃/min, and roasting for 2 hours to obtain a modified carrier;
(2) Preparation of the catalyst: 10g of the modified support was immersed in 80g of an aqueous slurry in which the mass fraction of copper nitrate was 12%, the mass fraction of zirconium nitrate was 5%, the mass fraction of expanded graphite was 25% and silica Sol (SiO) 2 25 wt.%) of 15%, ultrasonic dipping for 1h, followed by purging with compressed air, drying at 100 ℃ and then drying in a muffle furnace at a rate of 3 ℃/minAnd heating to 550 ℃ and roasting for 2 hours to obtain the catalyst.
Comparative example 1
The preparation method of the catalyst for purifying the tail gas of the explosion-proof diesel engine comprises the following steps:
a 10g Y type molecular sieve support was immersed in 80g of an aqueous slurry in which the mass fraction of copper nitrate was 12%, the mass fraction of zirconium nitrate was 5%, the mass fraction of expanded graphite was 25%, and silica sol (SiO 2 The mass fraction of the catalyst is 15 percent, the catalyst is immersed for 1h by ultrasonic, then the catalyst is purged by compressed air, dried at 100 ℃, and then baked for 2h after being heated to 550 ℃ in a muffle furnace at a speed of 3 ℃/min.
Comparative example 2
The preparation method of the catalyst for purifying the tail gas of the explosion-proof diesel engine comprises the following steps:
(1) Preparation of modified carrier: placing a 16g Y type molecular sieve carrier in 120g of mixed solution (the mass fraction of aluminum nitrate is 13% and the mass fraction of cerium nitrate is 21%), adding 4g of polyethylene glycol 400, stirring and mixing uniformly, dripping 1mol/L ammonia water to adjust the pH of the solution to 9, placing the solution in a crystallization kettle, reacting for 24 hours at 160 ℃, centrifuging, washing, drying and grinding after the reaction is finished, heating to 500 ℃ in a muffle furnace at a speed of 3 ℃/min, and roasting for 2 hours to obtain a modified carrier;
(2) Preparation of the catalyst: 10g of the modified support was immersed in 80g of an aqueous slurry in which the mass fraction of copper nitrate was 12%, the mass fraction of zirconium nitrate was 5% and silica sol (SiO 2 The mass fraction of the catalyst is 15 percent, the catalyst is immersed for 1h by ultrasonic, then the catalyst is purged by compressed air, dried at 100 ℃, and then baked for 2h after being heated to 550 ℃ in a muffle furnace at a speed of 3 ℃/min.
The catalysts prepared in examples 1-3 and comparative examples 1-2 were tested for performance by the following procedure:
0.5g of the catalysts prepared in examples 1 to 3 and comparative examples 1 to 2 were respectively charged into a quartz tube having an inner diameter of 10mm and a length of 400mm, and the reaction temperature was set200 ℃ and simulating diesel engine tail gas: 5000ppm CO+10% O 2 +10％H 2 O+200ppmSO 2 +N 2 Airspeed of 20000hr -1 The sulfur resistance of the catalyst was tested under this condition and the experimental results are shown in the following table:
finally, it should be noted that: the above examples are not intended to limit the present invention in any way. Modifications and improvements will readily occur to those skilled in the art upon the basis of the present invention. Accordingly, any modification or improvement made without departing from the spirit of the invention is within the scope of the invention as claimed.
Claims (10)
1. The preparation method of the catalyst for purifying the tail gas of the explosion-proof diesel engine is characterized by comprising the following steps of:
(1) Preparation of modified carrier: placing the Y-type molecular sieve carrier into a mixed solution of aluminum nitrate and cerium nitrate, adding polyethylene glycol, stirring and mixing uniformly, dripping ammonia water to adjust the pH value of the solution to 9-10, placing the solution into a crystallization kettle for reaction, and centrifuging, washing, drying, grinding and roasting after the reaction is completed to obtain a modified carrier;
(2) Preparation of the catalyst: immersing the modified carrier in aqueous slurry containing copper nitrate, zirconium nitrate, expanded graphite and silica sol, carrying out ultrasonic immersion for 1-2h, then blowing with compressed air, drying and roasting to obtain the catalyst.
2. The method for preparing a catalyst according to claim 1, wherein in the step (1), the mass ratio of the Y-type molecular sieve carrier, the mixed solution and the polyethylene glycol is 10-20:100-150:3-6.
3. The method for preparing a catalyst according to claim 1, wherein in the step (1), the mass fraction of aluminum nitrate is 12-14% and the mass fraction of cerium nitrate is 21-22%.
4. The method for preparing a catalyst according to claim 1, wherein in the step (1), the reaction temperature is 150 to 180 ℃ and the reaction time is 24 to 36 hours.
5. The method for preparing a catalyst according to claim 1, wherein in the step (2), the mass ratio of the modified support to the aqueous slurry is 1:4-8.
6. The method for preparing a catalyst according to claim 1, wherein in the step (2), the mass fraction of copper nitrate in the aqueous slurry is 10-15%, the mass fraction of zirconium nitrate is 4-8%, the mass fraction of expanded graphite is 20-30%, and the mass fraction of silica sol is 12-18%.
7. The method for preparing a catalyst according to claim 6, wherein SiO in the silica sol 2 The content of (C) is 25-30wt%.
8. The method for preparing a catalyst according to claim 1, wherein in the step (2), the calcination temperature is 500 to 550 ℃ and the calcination time is 2 to 4 hours.
9. A catalyst prepared by the method of any one of claims 1-8.
10. Use of the catalyst according to claim 9 for the purification of exhaust gases from explosion-proof diesel engines.
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