CN115962033A - Aftertreatment system for hydrogen internal combustion engine and alcohol internal combustion engine and preparation method thereof - Google Patents
Aftertreatment system for hydrogen internal combustion engine and alcohol internal combustion engine and preparation method thereof Download PDFInfo
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- CN115962033A CN115962033A CN202211645506.9A CN202211645506A CN115962033A CN 115962033 A CN115962033 A CN 115962033A CN 202211645506 A CN202211645506 A CN 202211645506A CN 115962033 A CN115962033 A CN 115962033A
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Abstract
The present invention relates to an aftertreatment system for an internal combustion engine, in particular for a hydrogen and alcohol internal combustion engine, and to a method for the production thereof. The system couples the DOC and the SCR and places the DOC function at the outlet end of the SCR to avoid NO x Contact with DOC while retaining alcohol and H 2 The oxidation function can also oxidize NH brought by over-injection of urea 3 . Control of catalysis through design of outlet end DOCThe strength of the whole oxidation function of the agent is strong and weak so as to meet the requirements of different applications.
Description
Technical Field
The present invention relates to an aftertreatment system for an internal combustion engine, in particular for a hydrogen and alcohol internal combustion engine, and to a method for the production thereof.
Background
Hydrogen energy is a clean energy source in the future. There are two ways of using mobile sources, hydrogen fuel cells and hydrogen internal combustion engines. Meanwhile, internal combustion engines using methanol and other fuels are also being actively propelled. The emission of hydrogen and methanol internal combustion engines is mainly NO x And unburned methanol, H 2 And formaldehyde, which is a reaction byproduct, and the like. A conventional system is DOC + SCR, where DOC is used for alcohol, H 2 Etc. oxidation, SCR for NO x While controlling N is also required 2 And (4) discharging O. The problem with conventional designs is the NO produced by the engine x DOC, NO through the front end x Part of NO in the catalyst is oxidized into NO by DOC 2 NO on downstream SCR 2 And reducing agent ammonia gas to easily generate N 2 O, resulting in control of N 2 The difficulty of O-discharge increases. There is therefore a need for improvements in aftertreatment systems and catalysts.
Disclosure of Invention
The object of the present invention is to provide a new aftertreatment system for hydrogen and alcohol internal combustion engines. The system couples the DOC and the SCR and places the DOC function at the outlet end of the SCR to avoid NO x Contact with DOC while retaining alcohol and H 2 The oxidation function can also oxidize NH brought by over-injection of urea 3 . The strength of the integral oxidation function of the catalyst is controlled by the design of the DOC at the outlet end so as to meet the requirements of different applications.
It is another object of the present invention to provide a method for preparing the above-described aftertreatment system.
The purpose of the invention is realized by the following technical scheme:
an aftertreatment system for hydrogen and alcohol internal combustion engines includes a carrier,
the inner wall of the carrier close to the outlet end is coated with a first noble metal catalyst coating containing noble metal components, and the length of the first noble metal catalyst coating is not less than 2/3 of the total length of the carrier; if the length is too short, the oxidation performance is insufficient, and if it is too long, NH3 is oxidized. The inner wall of the carrier close to the inlet end is coated with a second catalyst coating with SCR function, and the second catalyst coating partially covers the first catalyst coating;
the first catalyst coating at the outlet end is also coated with a third catalyst coating containing a noble metal component, and a gap is formed between the third catalyst coating and the second catalyst coating; the noble metal concentration in the third catalyst coating layer is greater than the noble metal concentration in the first catalyst coating layer.
Further, the covering length of the second catalyst coating layer partially covering the first catalyst coating layer is not less than 25mm. If the second layer of SCR overlaps the first layer too short, NH3 will be oxidized to Nox and not to N2.
Further, the ratio of the concentration of the noble metal in the third catalyst coating to the first catalyst coating is greater than 1.2.
Further, the second catalyst coating layer having the SCR function is a single coating layer having a uniform composition, or a plurality of coating layers having different compositions.
Further, the second catalyst coating with SCR function comprises a Cu-CHA zeolite coating, an Fe-Beta zeolite coating or a W-V-TiO coating 2 And (4) coating.
Further, the noble metal of the first catalyst coating layer is Pt, and the noble metal of the third catalyst coating layer is Pt and/or Pd.
Further, the gap between the third catalyst coating layer and the second catalyst coating layer is less than 10mm.
The preparation method of the aftertreatment system for the hydrogen internal combustion engine and the alcohol internal combustion engine comprises the following steps:
s1, preparation of first catalyst coating
Mixing a platinum nitrate solution and alumina slurry, adjusting viscosity and solid content, coating the slurry on a carrier, wherein the coating length is not less than 2/3 of the total length of the carrier, and controlling the concentration of Pt to be 1-3g/ft by controlling the coating amount 3 Drying at 100-150 deg.C, calcining at 500-600 deg.C to form a first catalyst coating layer on the side of the carrier at the outlet end;
s2, preparation of second catalyst coating
Adding water into the SCR coating slurry, uniformly stirring, adding a zirconium oxide adhesive, adding water to adjust the viscosity and solid content, wherein the coating amount is 80-140g/L based on the dry weight of the slurry, and the coating length is required to partially cover a first catalyst coating; drying at 100-150 deg.C, calcining at 500-600 deg.C to form a second catalyst coating layer on the side of the inlet end carrier;
s3, preparation of third catalyst coating
Mixing the components in a concentration ratio of 1:0 to 1:1, adjusting viscosity and solid content, coating from an outlet end, controlling the total concentration of Pt and Pd to be greater than the concentration of noble metal of the first catalyst coating by controlling the coating amount, ensuring the coating length to have a gap with the second catalyst coating, drying at 100-150 ℃, calcining at 500-600 ℃ to form a third catalyst coating of the outlet end.
Further, in the second catalyst coating preparation of step S2, one to more layers of other components of the coating layer having the SCR function are applied.
Further, the SCR coating slurry in the step S2 comprises Cu-CHA zeolite and/or Fe-Beta zeolite and/or W-V-TiO.
Further, the total concentration of Pt and Pd in the step S3 is 5-15g/ft 3 。
The invention has the following beneficial effects:
the system couples the DOC and the SCR and places the DOC function at the outlet end of the SCR to avoid NO x Contact with DOC while retaining alcohol and H 2 The oxidation function can also oxidize NH brought by over-injection of urea 3 . The strength of the integral oxidation function of the catalyst is controlled by the design of the DOC at the outlet end so as to meet the requirements of different applications.
Detailed Description
The present invention will be described in further detail with reference to specific examples and comparative examples.
Example 1
A hydrogen internal combustion engine and alcohol internal combustion engine after-treatment system, its preparation method is:
s1, mixing a platinum nitrate solution with the alumina slurry, and adjusting the viscosity and the solid content. The slurry was coated onto a blank ceramic honeycomb carrier,the carrier was 150mm x 150mm x 150mm, mesh 200, wall thickness 4mm. Coating a length of 100mm from the outlet end, and controlling the concentration of Pt to be 2g/ft by controlling the coating amount 3 Dried at a temperature of 100 to 150 ℃ and calcined at a temperature of 550 ℃ to form the noble metal catalyst on the side of the carrier at the outlet end.
S2, adding water into the Cu-CHA zeolite containing 3.0 percent of Cu, uniformly stirring, adding a zirconia binder, adding water to adjust the viscosity and the solid content, coating the mixture from an inlet end by a length of 100mm, and coating the mixture by 100g/L based on the dry weight of the slurry; dried at a temperature of 100-150 c and calcined at a temperature of 550 c to form the inlet end carrier side Cu-SCR catalyst.
S3, mixing a platinum nitrate solution, palladium acetate and alumina slurry, adjusting the viscosity and solid content, coating the mixture from an outlet end to a length of 40mm, and controlling the concentration of Pt to be 5g/ft by controlling the coating amount 3 The concentration of Pd is 2g/ft 3 . Dried at a temperature of 100-150 c and calcined at a temperature of 550 c to form the outlet end second layer noble metal catalyst.
Example 2
A hydrogen internal combustion engine and alcohol internal combustion engine after-treatment system, its preparation method is:
s1, mixing a platinum nitrate solution and the alumina slurry, and adjusting the viscosity and the solid content. The slurry was applied to a blank ceramic honeycomb carrier of 150mm x 150mm x 150mm x 150mm, mesh number 200, and wall thickness 4mm. The length of 100mm was coated from the outlet end, and the concentration of Pt was controlled to 2g/ft by controlling the coating amount 3 Dried at a temperature of 100 to 150 ℃ and calcined at a temperature of 550 ℃ to form the noble metal catalyst on the side of the carrier at the outlet end.
S2, adding water to Cu-CHA zeolite containing Cu 3.0% and stirring, adding zirconia binder, adding water to adjust viscosity and solid content, coating with a length of 90mm from the inlet end, and coating in an amount of 100g/L based on the dry weight of the slurry; dried at a temperature of 100-150 c and calcined at a temperature of 550 c to form the inlet end carrier side Cu-SCR catalyst.
S3, adding water into Fe-Beta zeolite containing 4.2wt% of Fe, uniformly stirring, then adding 15wt% of aqueous alumina, and adding water to adjust viscosity and solid content; coating the slurry from an inlet end, wherein the length of the slurry is 100mm respectively, so as to ensure that the Cu-SCR catalyst on the inlet side of the carrier can be covered by the Fe-beta slurry, and the coating amount is 120g/L based on the dry weight of the slurry; dried at a temperature of 100-150 c and calcined at a temperature of 550 c to form the second layer of the SCR catalyst at the inlet end.
S4, mixing a platinum nitrate solution, palladium acetate and alumina slurry, adjusting the viscosity and solid content, coating the mixture from an outlet end to a length of 40mm, and controlling the concentration of Pt to be 5g/ft by controlling the coating amount 3 The concentration of Pd is 2g/ft 3 . Dried at a temperature of 100-150 c and calcined at a temperature of 550 c to form a second layer of noble metal catalyst on the outlet end.
Example 3
A hydrogen internal combustion engine and alcohol internal combustion engine after-treatment system, its preparation method is:
s1, mixing a platinum nitrate solution and the alumina slurry, and adjusting the viscosity and the solid content. The slurry was coated onto a blank ceramic honeycomb support of 150mm x 150mm x 150mm, mesh 200 and wall thickness 4mm. Coating a length of 100mm from the outlet end, and controlling the concentration of Pt to be 2g/ft by controlling the coating amount 3 Dried at a temperature of 100 to 150 c and calcined at a temperature of 550 c to form the noble metal catalyst on the side of the outlet-end carrier.
S2, coating the SCR slurry containing 2.5 percent V of W-V-TiO2 at the inlet end for 100mm after adjusting the viscosity and the solid content; the coated amount was 240g/L based on dry weight of the slurry, dried at a temperature of 100-150 ℃ and calcined at a temperature of 550 ℃ to form the V-SCR catalyst on the inlet end carrier side.
S3, mixing a platinum nitrate solution, palladium acetate and alumina slurry, adjusting viscosity and solid content, coating the mixture from an outlet end for 40mm in length, and controlling the concentration of Pt to be 5g/ft by controlling the coating amount 3 The concentration of Pd is 2g/ft 3 . Dried at a temperature of 100-150 c and calcined at a temperature of 550 c to form a second layer of noble metal catalyst on the outlet end.
Comparative example 1
A hydrogen internal combustion engine and alcohol internal combustion engine after-treatment system, its preparation method is:
s1, mixing a platinum nitrate solution and the alumina slurry, and adjusting the viscosity and the solid content. The slurry was coated onto a blank ceramic honeycomb support of 150mm x 150mm x 150mm, mesh 200 and wall thickness 4mm. Coating a length of 100mm from the outlet end, and controlling the concentration of Pt to be 2g/ft by controlling the coating amount 3 Dried at a temperature of 100 to 150 ℃ and calcined at a temperature of 550 ℃ to form the noble metal catalyst on the side of the carrier at the outlet end.
S2, adding water to Cu-CHA zeolite containing Cu 3.0% and stirring, adding zirconia binder, adding water to adjust viscosity and solid content, coating with 100mm length from inlet end, and coating with 100g/L based on dry weight of slurry; after drying at 100 to 150 ℃, the slurry was coated from the outlet end in the same manner so as to have a length of 100mm, the amount of coating was 100g/L based on the dry weight of the slurry, and after drying at 100 to 150 ℃, the slurry was calcined at 550 ℃ to obtain a Cu-SCR catalyst. The Cu-SCR completely covered the noble metal catalyst on the side of the outlet end support.
Comparative example 2
A hydrogen internal combustion engine and alcohol internal combustion engine after-treatment system, its preparation method is:
s1, mixing a platinum nitrate solution with the alumina slurry, and adjusting the viscosity and the solid content. The slurry was coated onto a blank ceramic honeycomb support of 150mm x 150mm x 150mm, mesh 200 and wall thickness 4mm. Coating a length of 100mm from the outlet end, and controlling the concentration of Pt to be 2g/ft by controlling the coating amount 3 Dried at a temperature of 100 to 150 c and calcined at a temperature of 550 c to form the noble metal catalyst on the side of the outlet-end carrier.
S2, adding water to Cu-CHA zeolite containing Cu 3.0% and stirring, adding zirconia binder, adding water to adjust viscosity and solid content, coating with a length of 110mm from the inlet end, and coating in an amount of 100g/L based on the dry weight of the slurry; after drying at a temperature of 100-150 c, calcination at a temperature of 550 c forms the inlet end carrier side Cu-SCR catalyst.
Comparative example 3
A hydrogen internal combustion engine and alcohol internal combustion engine after-treatment system, its preparation method is:
s1, mixing a platinum nitrate solutionAnd mixing with alumina slurry to regulate viscosity and solid content. The slurry was coated onto a blank ceramic honeycomb support of 150mm x 150mm x 150mm, mesh 200 and wall thickness 4mm. Coating a length of 100mm from the outlet end, and controlling the concentration of Pt to be 8 g/ft by controlling the coating amount 3 Dried at a temperature of 100 to 150 c and calcined at a temperature of 550 c to form the noble metal catalyst on the side of the outlet-end carrier.
S2, adding water into the Cu-CHA zeolite containing 3.0 percent of Cu, uniformly stirring, adding a zirconia binder, adding water to adjust the viscosity and the solid content, coating the mixture from an inlet end by a length of 110mm, and coating the mixture by 100g/L based on the dry weight of the slurry; after drying at a temperature of 100-150 c, calcination at a temperature of 550 c forms the inlet end carrier side Cu-SCR catalyst.
Comparative example 4
A hydrogen internal combustion engine and alcohol internal combustion engine after-treatment system, its preparation method is:
s1, mixing a platinum nitrate solution, platinum acetate and alumina slurry, and adjusting viscosity and solid content. The slurry was coated onto a blank ceramic honeycomb support of 150mm x 150mm x 150mm, mesh 200 and wall thickness 4mm. Coating a length of 100mm from the outlet end, and controlling the concentration of Pt to be 7 g/ft by controlling the coating amount 3 The concentration of Pd is 2g/ft 3 . Drying at a temperature of 100-150 ℃ and calcining at a temperature of 550 ℃ to form the noble metal catalyst on the side of the carrier at the outlet end.
S2, adding water into the Cu-CHA zeolite containing 3.0 percent of Cu, uniformly stirring, adding a zirconia binder, adding water to adjust the viscosity and the solid content, coating the mixture from an inlet end by a length of 110mm, and coating the mixture by 100g/L based on the dry weight of the slurry; after drying at a temperature of 100-150 c, calcination was carried out at a temperature of 550 c to form the inlet end carrier side Cu-SCR catalyst.
Comparative example 5
A hydrogen internal combustion engine and alcohol internal combustion engine after-treatment system, its preparation method is:
s1, mixing a platinum nitrate solution, platinum acetate and alumina slurry, and adjusting viscosity and solid content. The slurry was coated onto a blank ceramic honeycomb carrier of 150mm x 150mm x 150mm x 150mm, mesh number 200,the wall thickness was 4mm. The length of 100mm was coated from the outlet end, and the concentration of Pt was controlled to be 7 g/ft by controlling the coating amount 3 The concentration of Pd is 2g/ft 3 . Drying at a temperature of 100-150 ℃ and calcining at a temperature of 550 ℃ to form the noble metal catalyst on the side of the carrier at the outlet end.
S2, coating the SCR slurry containing 2.5 percent V of W-V-TiO2 at the inlet end for 100mm after adjusting the viscosity and the solid content; the coated amount was 240g/L based on dry weight of the slurry, dried at a temperature of 100-150 deg.C, and calcined at a temperature of 550 deg.C to form an inlet end carrier side V-SCR catalyst.
Examples and comparative examples performance test methods and test data:
a 1 inch diameter and 3 inch long sample was taken from the catalyst sample and tested for performance using a simulated gas. The gas conditions are shown in table 1 below. Mainly considers the NOx conversion efficiency and the concentration of harmful byproduct N2O in SCR reaction, and simultaneously utilizes the conversion efficiency of CO/H2 to consider the oxidation performance of the catalyst.
Table 1 test conditions (concentration units are ppm without indication):
the results of examples 1,2 and comparative examples 1 to 4 are shown in the following table
Comparison of catalyst Performance (200 degree)
Comparison of catalyst Performance (500 degree)
From the results of examples 1 and 2 and comparative example 1, it can be seen that the NOx conversion efficiencies of the two are close, but the H2 conversion efficiency of the example is higher than that of comparative example 1, and the N2O concentration is lower. Since the high concentration of noble metal in the examples is mainly distributed at the outlet side, the influence on the SCR reaction is small.
From the results of examples 1,2 and comparative example 2, it can be seen that the catalytic component of SCR in comparative example 2 is high, and therefore NOx is generated
The conversion efficiency is better, but the emission of high concentrations of N2O is caused by the higher concentration of precious metals in the DOC portion of the bottom layer. Thus by increasing the base DOC precious metal concentration, higher H2/CO conversion efficiencies can be achieved, but also higher N2O emissions.
From the results of examples 1,2 and comparative examples 3,4, the NOx conversion efficiencies of the SCRs are similar, and the CO/H2 oxidizing abilities are also close, but the N2O concentrations of examples 1,2 are significantly lower.
Therefore, the design of the embodiment 1 and 2 ensures the conversion efficiency of NOx in SCR reaction, and the design of the DOC with high outlet concentration effectively inhibits the generation of N2O on the premise of not influencing the oxidation performance of CO/H2.
In example 3, V-SCR coating was used. Comparing with comparative example 5, the conversion efficiency of NOx, CO/H2 of the example is close to that of comparative example 5, but the concentration of N2O is obviously lower. Therefore, the effect of the design is insensitive to different SCR catalysts and can be applied to different SCRs.
Comparison of catalyst Performance (200 degree)
Comparison of catalyst Performance (500 degree)
While the invention has been described in conjunction with the specific embodiments set forth above, it is evident that many alternatives, modifications, and variations will be apparent to those skilled in the art in light of the foregoing description. Accordingly, it is intended to embrace all such alternatives, modifications and variations that fall within the spirit and scope of the appended claims.
Claims (10)
1. An aftertreatment system for hydrogen and alcohol internal combustion engines comprising a carrier, characterized by:
the inner wall of the carrier close to the outlet end is coated with a first catalyst coating containing precious metal components, and the length of the first catalyst coating is not less than 2/3 of the total length of the carrier;
the inner wall of the carrier close to the inlet end is coated with a second catalyst coating with SCR function, and the second catalyst coating partially covers the first catalyst coating;
the first catalyst coating at the outlet end is also coated with a third catalyst coating containing a noble metal component, and a gap is formed between the third catalyst coating and the second catalyst coating; the noble metal concentration in the third catalyst coating layer is greater than the noble metal concentration in the first catalyst coating layer.
2. The aftertreatment system for hydrogen and alcohol internal combustion engines according to claim 1, wherein: the covering length of the second catalyst coating layer partially covering the first catalyst coating layer is not less than 25mm.
3. The aftertreatment system for a hydrogen internal combustion engine and an alcohol internal combustion engine according to claim 1, characterized in that: the ratio of the noble metal concentration in the third catalyst coating to the first catalyst coating is greater than 1.2.
4. The aftertreatment system for a hydrogen internal combustion engine and an alcohol internal combustion engine according to claim 1, characterized in that: the second catalyst coating with the SCR function is a coating with a uniform component or a plurality of coatings with different components.
5. The aftertreatment system for hydrogen and alcohol internal combustion engines according to claim 4, wherein: the second catalyst coating with the SCR function comprises a Cu-CHA zeolite coating, an Fe-Beta zeolite coating or a W-V-TiO 2 And (4) coating.
6. The aftertreatment system for a hydrogen internal combustion engine and an alcohol internal combustion engine according to claim 1, characterized in that: the noble metal of the first catalyst coating layer is Pt and the noble metal of the third catalyst coating layer is Pt and/or Pd.
7. A method of producing the aftertreatment system for hydrogen internal combustion engines and alcohol internal combustion engines according to any one of claims 1 to 6, characterized by comprising the steps of:
s1, preparation of first catalyst coating
Mixing a platinum solution and an alumina slurry, adjusting viscosity and solid content, coating the slurry on a carrier, wherein the coating length is not less than 2/3 of the total length of the carrier, and controlling the concentration of Pt to be 1-3g/ft by controlling the coating amount 3 Drying at 100-150 deg.C, calcining at 500-600 deg.C to form a first catalyst coating layer on the side of the carrier at the outlet end;
s2, preparation of second catalyst coating
Adding water into the SCR coating slurry, uniformly stirring, adding a zirconium oxide adhesive, adding water to adjust the viscosity and solid content, wherein the coating amount is 80-140g/L based on the dry weight of the slurry, and the coating length is required to partially cover a first catalyst coating; drying at 100-150 deg.C, calcining at 500-600 deg.C to form a second catalyst coating layer on the side of the inlet end carrier;
s3, preparation of third catalyst coating
Mixing the components in a concentration ratio of 1:0 to 1:1, adjusting viscosity and solid content, coating from an outlet end, controlling the total concentration of Pt and Pd to be more than the concentration of noble metal of the first catalyst coating by controlling the coating amount, ensuring that a gap is reserved between the coating length and the second catalyst coating, drying at the temperature of 100-150 ℃, and calcining at the temperature of 500-600 ℃ to form a third catalyst coating at the outlet end.
8. The production method of an aftertreatment system for a hydrogen internal combustion engine and an alcohol internal combustion engine according to claim 7, characterized in that: step S2, in the preparation of the second catalyst coating layer, one to more layers of other components of the coating layer having the SCR function are applied.
9. The production method of an aftertreatment system for a hydrogen internal combustion engine and an alcohol internal combustion engine according to claim 7, characterized in that: the SCR coating slurry in the step S2 comprises Cu-CHA zeolite and/or Fe-Beta zeolite and/or W-V-TiO.
10. The production method of an aftertreatment system for a hydrogen internal combustion engine and an alcohol internal combustion engine according to claim 7, characterized in that: the total concentration of Pt and Pd in the step S3 is 5-15g/ft 3 。
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