CN103191734A - Three-element catalyst for treating automobile exhaust - Google Patents
Three-element catalyst for treating automobile exhaust Download PDFInfo
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- CN103191734A CN103191734A CN2013100837420A CN201310083742A CN103191734A CN 103191734 A CN103191734 A CN 103191734A CN 2013100837420 A CN2013100837420 A CN 2013100837420A CN 201310083742 A CN201310083742 A CN 201310083742A CN 103191734 A CN103191734 A CN 103191734A
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- lower floor
- way catalyst
- vehicle exhaust
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Abstract
The invention relates to a three-way catalyst for treating automobile exhaust. The three-way catalyst comprises a honeycomb-like carrier and is characterized in that a lower Pd coating is attached on the honeycomb-like carrier, a middle Pd coating is attached on the lower Pd coating, an upper Rh coating is attached on the middle Pd coating, wherein the lower Pd coating comprises a Pd-loaded cerium-zirconium solid solution and La2O3-doped aluminum oxide (La2O3-Al2O3), the middle Pd coating comprises Pd-loaded La2O3-Al2O3 and a binding agent, and the upper Rh coating comprises Rh-loaded cerium-zirconium solid solution and the La2O3-Al2O3. As for the three-way catalyst disclosed by the invention, as the middle Pd coating does not contain a CeO2 component and Pd is loaded on the La2O3-Al2O3, the catalytic ability of the catalyst is improved and the oxygen storage ability of the catalyst is improved; and compared with a traditional Pd/Rh double-coating three-element catalyst, the three-element catalyst disclosed by the invention has higher ability of processing hydrocarbons, carbon monoxide and nitrogen oxides, and especially has higher ability of transforming the nitrogen oxides.
Description
Technical field
The present invention relates to a kind of three-way catalyst for the vehicle exhaust processing,, belong to the purifying vehicle exhaust technical field.
Background technology
The major pollutants of vehicle exhaust are carbon monoxide (CO), hydrocarbon (HC) and oxynitrides (NOx), utilize the catalyst that is installed in gas extraction system carbon monoxide, oxidizing hydrocarbon can be become carbon dioxide (CO
2), water (H
2O), and simultaneously make oxynitrides be reduced to nitrogen (N
2), realize the purification of tail gas, this catalyst is commonly referred to three-way catalyst.Three-way catalyst is made up of two parts: cellular pottery or metallic carrier, and be attached to the supported catalyst coating.Catalyst coat is usually by having oxide material (as aluminium oxide), the hydrogen-storing material than bigger serface and being dispersed in oxide or the noble metal active component on hydrogen-storing material surface (often for Pt(platinum), Pd(palladium), the Rh(rhodium) in one or more) form.Hydrogen-storing material wherein is generally the composite oxides that contain the cerium zirconium, it stores the oxygen in the tail gas by absorption or discharges the ratio that oxygen is regulated oxidisability component and reproducibility component in the tail gas, and oxynitrides is reduced when making carbon monoxide and hydrocarbon oxidized.The transformation efficiency of pollutant when improving cold-starting automobile, three-way catalyst often is installed in the position near the enmgine exhaust outlet, and when galloping, the bed temperature of three-way catalyst can reach 900 ℃ ~ 1100 ℃ high temperature.
Mainly make catalyst activity reduction for the alloying action that suppresses Rh and Pd under the hot conditions, present three-way catalyst all adopts two coating structures usually, namely be attached to the following coating loading Pd on the honeycomb substrate, coating material generally comprises cerium zirconium sosoloid, aluminium oxide and other auxiliary agents; And the last coating that is attached to down on the coating supports Rh, and coating material generally also comprises cerium zirconium sosoloid, aluminium oxide and other auxiliary agents.Yet under high-temperature oxygen-enriched condition, the easily downward coating of the Rh of last coating is moved and is interacted with Pd, and activity of such catalysts is descended.In addition, Rh loads on oxygen storage capacity is significantly improved, still, hydrogen-storing material store the easier oxidation state that is in of Rh that the oxygen function makes its load, and the activity of the Rh catalysis oxynitrides of oxidation state reduction is very low, even at motor exhaust by rare transient condition that thickens.
Summary of the invention
The objective of the invention is to overcome the deficiencies in the prior art, a kind of three-way catalyst for the vehicle exhaust processing is provided, have higher hydrocarbon, carbon monoxide and oxynitrides disposal ability, it suppresses Rh to the migration of Pd coating, has improved the activity of Rh catalytic reduction oxynitrides.
According to technical scheme provided by the invention, described three-way catalyst for the vehicle exhaust processing comprises honeycomb support, it is characterized in that: adhere to the Pd of lower floor coating at described honeycomb support, the Pd coating is adhered to upper strata Rh coating in middle Pd coating in the middle of lower floor's Pd coating is adhered to; The described Pd of lower floor coating comprises cerium zirconium sosoloid and the La of load P d
2O
3Aluminium oxide (the La that mixes
2O
3-Al
2O
3), middle Pd coating comprises the La of load P d
2O
3-Al
2O
3And binding agent, upper strata Rh coating comprises cerium zirconium sosoloid and the La of load Rh
2O
3-Al
2O
3
In a specific embodiment, in the described Pd of the lower floor coating, the cerium zirconium sosoloid of load P d and La
2O
3-Al
2O
3Mass ratio be 1 ~ 3:1.
In a specific embodiment, in the described middle Pd coating, the 1wt% ~ 10wt% of Pd coating gross mass in the middle of binding agent accounts for.
In a specific embodiment, in the Rh coating of described upper strata, the cerium zirconium sosoloid of load Rh and La
2O
3-Al
2O
3Mass ratio be 2 ~ 5:1.
In a specific embodiment, the component of described cerium zirconium sosoloid is: the ZrO of 20wt% ~ 70wt%
2, 20wt% ~ 70wt% CeO
2And the La of 10wt% ~ 15wt%
2O
3, Y
2O
3, Pr6O
11, Nd
2O
3In one or more.
In a specific embodiment, the load capacity of Pd is 5 ~ 200g/ft in the described Pd of the lower floor coating
3, the load capacity of Pd is 5 ~ 200g/ft in the middle Pd coating
3, the load capacity of Rh is 0.1 ~ 10g/ft in the Rh coating of upper strata
3
In a specific embodiment, the mass ratio of the Pd of load is 3:1 ~ 9 in the described Pd of lower floor coating and the middle Pd coating.
In a specific embodiment, the coated weight of the described Pd of lower floor coating is 30 ~ 100g/L, and the coated weight of middle Pd coating is 30 ~ 100g/L, upper strata Rh coating be applied to 50 ~ 160g/L.
In a specific embodiment, described La
2O
3-Al
2O
3In La
2O
3Content accounts for La
2O
3-Al
2O
32wt% ~ 10wt%.
In a specific embodiment, described binding agent is ZrO
2
Advantage of the present invention is: (1) three-way catalyst of the present invention is Pd/Pd/Rh three coating structures, owing to do not contain CeO in the middle Pd coating
2Component has suppressed the migration of upper strata Rh to middle Pd coating; (2) three-way catalyst of the present invention is not owing to contain CeO in the middle Pd coating
2Component, and Pd loads on La
2O
3-Al
2O
3On, improved the catalytic capability of catalyst; (3) Pd is supported on the cerium zirconium sosoloid in the Pd of the lower floor coating of three-way catalyst of the present invention, has improved the oxygen storage capacity of catalyst; (4) three-way catalyst of the present invention is compared with the two coating three-way catalysts of traditional Pd/Rh, has higher hydrocarbon, carbon monoxide and oxynitrides disposal ability, especially has higher oxynitrides conversion capability.
The specific embodiment
The invention will be further described below in conjunction with specific embodiment.
Embodiment 1: a kind of three-way catalyst for the vehicle exhaust processing, comprise honeycomb support, and specification is Ф 118.4mm * 152.4mm, and Kong Mi counts 600cpsi, and the duct wall thickness is 4.3mil, and volume is 1.678L; Adhere to the Pd of lower floor coating at described honeycomb support, the Pd coating is adhered to upper strata Rh coating in middle Pd coating in the middle of lower floor's Pd coating is adhered to; The described Pd of lower floor coating comprises cerium zirconium sosoloid and the La of load P d
2O
3Aluminium oxide (the La that mixes
2O
3-Al
2O
3), middle Pd coating comprises the La of load P d
2O
3-Al
2O
3And ZrO
2, upper strata Rh coating comprises cerium zirconium sosoloid and the La of load Rh
2O
3-Al
2O
3The load capacity of Pd is 18g/ft in the described Pd of the lower floor coating
3, the load capacity of Pd is 18g/ft in the middle Pd coating
3, the load capacity of Rh is 4g/ft in the Rh coating of upper strata
3
The preparation method of described three-way catalyst, adopt following processing step:
The coating procedure of the 1st step, the described Pd of lower floor coating: with the cerium zirconium sosoloid of 1000g load P d, the La of 500g
2O
3-Al
2O
3(La
2O
3-Al
2O
3In La
2O
3Content accounts for La
2O
3-Al
2O
34wt%) and appropriate amount of deionized water mix, and preparation obtains the coating slurries behind ball milling; These coating slurries are coated on the honeycomb support, and the coated weight of the Pd of lower floor coating is 60g/L, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtains lower floor's coating; Wherein, the component of cerium zirconium sosoloid is: the ZrO of 45wt%
2, 45wt% CeO
2, 5wt% La
2O
3Pr6O with 5wt%
11
The coating procedure of the 2nd step, described middle Pd coating: with the La of 1000g load P d
2O
3-Al
2O
3(La
2O
3-Al
2O
3In La
2O
3Content accounts for La
2O
3-Al
2O
34wt%), the 400 zirconium oxyacetate solution (ZrO that contain 84g
2) and the appropriate amount of deionized water mixing, and preparation obtains the coating slurries behind ball milling; These coating slurries are coated on the 1st honeycomb support of step after finishing, and the coated weight of middle Pd coating is 60g/L, and in 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, Pd coating in the middle of obtaining;
The coating procedure of the 3rd step, described upper strata Rh coating: with the cerium zirconium sosoloid of 900g load Rh, the La of 300g
2O
3-Al
2O
3(La
2O
3-Al
2O
3In La
2O
3Content accounts for La
2O
3-Al
2O
34wt%) and appropriate amount of deionized water mix, and preparation obtains the coating slurries behind ball milling; These coating slurries are coated on the 2nd honeycomb support of step after finishing, upper strata Rh coating be applied to 100g/L, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtain upper strata Rh coating; Wherein, the component of cerium zirconium sosoloid is: the ZrO of 45wt%
2, 45wt% CeO
2, 5wt% La
2O
3And 5wt%Nd
2O
3
Embodiment 2: a kind of three-way catalyst for the vehicle exhaust processing, comprise honeycomb support, and specification is Ф 118.4mm * 152.4mm, and Kong Mi counts 600cpsi, and the duct wall thickness is 4.3mil, and volume is 1.678L; Adhere to the Pd of lower floor coating at described honeycomb support, the Pd coating is adhered to upper strata Rh coating in middle Pd coating in the middle of lower floor's Pd coating is adhered to; The described Pd of lower floor coating comprises cerium zirconium sosoloid and the La of load P d
2O
3Aluminium oxide (the La that mixes
2O
3-Al
2O
3), middle Pd coating comprises the La of load P d
2O
3-Al
2O
3And ZrO
2, upper strata Rh coating comprises cerium zirconium sosoloid and the La of load Rh
2O
3-Al
2O
3The load capacity of Pd is 15g/ft in the described Pd of the lower floor coating
3, the load capacity of Pd is 5g/ft in the middle Pd coating
3, the load capacity of Rh is 0.1g/ft in the Rh coating of upper strata
3
The preparation method of described three-way catalyst, adopt following processing step:
The coating procedure of the 1st step, the described Pd of lower floor coating: with the cerium zirconium sosoloid of 1000g load P d, the La of 1000g
2O
3-Al
2O
3(La
2O
3-Al
2O
3In La
2O
3Content accounts for La
2O
3-Al
2O
32wt%) and appropriate amount of deionized water mix, and preparation obtains the coating slurries behind ball milling; These coating slurries are coated on the honeycomb support, and the coated weight of the Pd of lower floor coating is 30g/L, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtains lower floor's coating; Wherein, the component of cerium zirconium sosoloid is: the ZrO of 20wt%
2, 60wt% CeO
2, 5wt% La
2O
3, 5wt% Y
2O
3, 5wt% Pr6O
11Nd with 5wt%
2O
3
The coating procedure of the 2nd step, described middle Pd coating: with the La of 1000g load P d
2O
3-Al
2O
3(La
2O
3-Al
2O
3In La
2O
3Content accounts for La
2O
3-Al
2O
32wt%), the 400 zirconium oxyacetate solution (ZrO that contain 84g
2) and the appropriate amount of deionized water mixing, and preparation obtains the coating slurries behind ball milling; These coating slurries are coated on the 1st honeycomb support of step after finishing, and the coated weight of middle Pd coating is 30g/L, and in 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, Pd coating in the middle of obtaining;
The coating procedure of the 3rd step, described upper strata Rh coating: with the cerium zirconium sosoloid of 900g load Rh, the La of 450g
2O
3-Al
2O
3(La
2O
3-Al
2O
3In La
2O
3Content accounts for La
2O
3-Al
2O
32wt%) and appropriate amount of deionized water mix, and preparation obtains the coating slurries behind ball milling; These coating slurries are coated on the 2nd honeycomb support of step after finishing, upper strata Rh coating be applied to 50 ~ 160g/L, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtain upper strata Rh coating; Wherein, the component of cerium zirconium sosoloid is: the ZrO of 20wt%
2, 60wt% CeO
2, 5wt% La
2O
3, 5wt% Y
2O
3, 5wt% Pr6O
11Nd with 5wt%
2O
3
Embodiment 3: a kind of three-way catalyst for the vehicle exhaust processing, comprise honeycomb support, and specification is Ф 118.4mm * 152.4mm, and Kong Mi counts 600cpsi, and the duct wall thickness is 4.3mil, and volume is 1.678L; Adhere to the Pd of lower floor coating at described honeycomb support, the Pd coating is adhered to upper strata Rh coating in middle Pd coating in the middle of lower floor's Pd coating is adhered to; The described Pd of lower floor coating comprises cerium zirconium sosoloid and the La of load P d
2O
3Aluminium oxide (the La that mixes
2O
3-Al
2O
3), middle Pd coating comprises the La of load P d
2O
3-Al
2O
3And ZrO
2, upper strata Rh coating comprises cerium zirconium sosoloid and the La of load Rh
2O
3-Al
2O
3The load capacity of Pd is 60g/ft in the described Pd of the lower floor coating
3, the load capacity of Pd is 180g/ft in the middle Pd coating
3, the load capacity of Rh is 10g/ft in the Rh coating of upper strata
3
The preparation method of described three-way catalyst, adopt following processing step:
The coating procedure of the 1st step, the described Pd of lower floor coating: with the cerium zirconium sosoloid of 900g load P d, the La of 300g
2O
3-Al
2O
3(La
2O
3-Al
2O
3In La
2O
3Content accounts for La
2O
3-Al
2O
310wt%) and appropriate amount of deionized water mix, and preparation obtains the coating slurries behind ball milling; These coating slurries are coated on the honeycomb support, and the coated weight of the Pd of lower floor coating is 100g/L, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtains lower floor's coating; Wherein, the component of cerium zirconium sosoloid is: the ZrO of 70wt%
2, 20wt% CeO
2, 5wt% La
2O
3Y with 5wt%
2O
3
The coating procedure of the 2nd step, described middle Pd coating: with the La of 1000g load P d
2O
3-Al
2O
3(La
2O
3-Al
2O
3In La
2O
3Content accounts for La
2O
3-Al
2O
310wt%), the 400 zirconium oxyacetate solution (ZrO that contain 84g
2) and the appropriate amount of deionized water mixing, and preparation obtains the coating slurries behind ball milling; These coating slurries are coated on the 1st honeycomb support of step after finishing, and the coated weight of middle Pd coating is 100g/L, and in 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, Pd coating in the middle of obtaining;
The coating procedure of the 3rd step, described upper strata Rh coating: with the cerium zirconium sosoloid of 900g load Rh, the La of 180g
2O
3-Al
2O
3(La
2O
3-Al
2O
3In La
2O
3Content accounts for La
2O
3-Al
2O
310wt%) and appropriate amount of deionized water mix, and preparation obtains the coating slurries behind ball milling; These coating slurries are coated on the 2nd honeycomb support of step after finishing, upper strata Rh coating be applied to 160g/L, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtain upper strata Rh coating; Wherein, the component of cerium zirconium sosoloid is: the ZrO of 70wt%
2, 20wt% CeO
2, 5wt% La
2O
3Y with 5wt%
2O
3
Comparative Examples 1: each parameter, composition and preparation process are identical with embodiment 1, and except not containing the middle Pd coating among the embodiment 1, and the coated weight of the Pd of lower floor coating becomes 120g/L, and the load capacity of Pd becomes 36g/ft
3
Comparative Examples 2: each parameter, composition and preparation process are identical with embodiment 1, and except not containing the Pd of the lower floor coating among the embodiment 1, and the coated weight of middle level Pd coating becomes 120g/L, and the load capacity of Pd becomes 36g/ft
3
With embodiment 1 and Comparative Examples 1 ~ Comparative Examples 2 resulting catalyst samples all according to the aging circulation of GMAC875 stand of General Motors Overseas Corporation with condition after aging 50 hours, adopt electron probe X ray micro-zone analysis instrument (EPMA) to analyze Rh in the distribution proportion situation of each coating of catalyst, the result is as shown in table 1.
Table 1
| ? | The Pd of lower floor coating | Middle Pd coating | Upper strata Rh coating |
| Embodiment 1 | 6% | 16% | 78% |
| Comparative Examples 1 | 41% | —— | 59% |
| Comparative Examples 2 | —— | 17% | 83% |
The car load emission test is undertaken by the ECE+EUDC circulation, the engine displacement 1.8L of testing vehicle, and the emission test result is as shown in table 2.
Table 2
| ? | Hydrocarbon (g/km) | Carbon monoxide (g/km) | Oxynitrides (g/km) |
| Embodiment 1 | 0.0436 | 0.689 | 0.0377 |
| Comparative Examples 1 | 0.0501 | 0.691 | 0.0580 |
| Comparative Examples 2 | 0.0477 | 1.013 | 0.0739 |
Shown in table, table 2, the result of catalyst performance test and evaluation shows, compare with Comparative Examples 1,2, the embodiment of the invention 1 disclosed three-way catalyst has suppressed the migration of Rh to the Pd layer, also possesses simultaneously high oxygen storage power, make catalyst have higher pollutant disposal ability, especially more excellent oxynitrides conversion capability.
Claims (10)
1. one kind is used for the three-way catalyst that vehicle exhaust is handled, and comprises honeycomb support, it is characterized in that: adhere to the Pd of lower floor coating at described honeycomb support, the Pd coating is adhered to upper strata Rh coating in middle Pd coating in the middle of lower floor's Pd coating is adhered to; The described Pd of lower floor coating comprises cerium zirconium sosoloid and the La of load P d
2O
3Aluminium oxide (the La that mixes
2O
3-Al
2O
3), middle Pd coating comprises the La of load P d
2O
3-Al
2O
3And binding agent, upper strata Rh coating comprises cerium zirconium sosoloid and the La of load Rh
2O
3-Al
2O
3
2. the three-way catalyst of handling for vehicle exhaust as claimed in claim 1 is characterized in that: in the described Pd of the lower floor coating, and the cerium zirconium sosoloid of load P d and La
2O
3-Al
2O
3Mass ratio be 1 ~ 3:1.
3. the three-way catalyst of handling for vehicle exhaust as claimed in claim 1 is characterized in that: in the middle of described in the Pd coating, and the 1wt% ~ 10wt% of Pd coating gross mass in the middle of binding agent accounts for.
4. the three-way catalyst of handling for vehicle exhaust as claimed in claim 1 is characterized in that: in the Rh coating of described upper strata, and the cerium zirconium sosoloid of load Rh and La
2O
3-Al
2O
3Mass ratio be 2 ~ 5:1.
5. as claim 2 or 4 described three-way catalysts for the vehicle exhaust processing, it is characterized in that: the component of described cerium zirconium sosoloid is: the ZrO of 20wt% ~ 70wt%
2, 20wt% ~ 70wt% CeO
2And the La of 10wt% ~ 15wt%
2O
3, Y
2O
3, Pr6O
11, Nd
2O
3In one or more.
6. the three-way catalyst of handling for vehicle exhaust as claimed in claim 1, it is characterized in that: the load capacity of Pd is 5 ~ 200g/ft in the described Pd of the lower floor coating
3, the load capacity of Pd is 5 ~ 200g/ft in the middle Pd coating
3, the load capacity of Rh is 0.1 ~ 10g/ft in the Rh coating of upper strata
3
7. the three-way catalyst of handling for vehicle exhaust as claimed in claim 6, it is characterized in that: the mass ratio of the Pd of load is 3:1 ~ 9 in the described Pd of lower floor coating and the middle Pd coating.
8. the three-way catalyst of handling for vehicle exhaust as claimed in claim 1, it is characterized in that: the coated weight of the described Pd of lower floor coating is 30 ~ 100g/L, the coated weight of middle Pd coating is 30 ~ 100g/L, upper strata Rh coating be applied to 50 ~ 160g/L.
9. as claim 2,3 or 4 described three-way catalysts for the vehicle exhaust processing, it is characterized in that: described La
2O
3-Al
2O
3In La
2O
3Content accounts for La
2O
3-Al
2O
32wt% ~ 10wt%.
10. the three-way catalyst of handling for vehicle exhaust as claimed in claim 1, it is characterized in that: described binding agent is ZrO
2
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|---|---|---|---|
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|---|---|---|---|
| CN201310083742.0A CN103191734B (en) | 2013-03-15 | 2013-03-15 | Three-element catalyst for treating automobile exhaust |
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| CN109310992A (en) * | 2016-06-07 | 2019-02-05 | 株式会社科特拉 | Exhaust gas purification catalyst |
| CN110756006A (en) * | 2019-07-10 | 2020-02-07 | 内蒙古中泰汇金环保科技有限公司 | Quenching absorption tower for treating waste gas generated by recycling hazardous waste inorganic salt |
| CN113231079A (en) * | 2021-05-26 | 2021-08-10 | 无锡威孚环保催化剂有限公司 | Ternary catalyst for enhancing automobile exhaust purification and preparation method thereof |
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| CN110756006A (en) * | 2019-07-10 | 2020-02-07 | 内蒙古中泰汇金环保科技有限公司 | Quenching absorption tower for treating waste gas generated by recycling hazardous waste inorganic salt |
| CN110756006B (en) * | 2019-07-10 | 2021-09-28 | 内蒙古中泰汇金环保科技有限公司 | Quenching absorption tower for treating waste gas generated by recycling hazardous waste inorganic salt |
| CN113231079A (en) * | 2021-05-26 | 2021-08-10 | 无锡威孚环保催化剂有限公司 | Ternary catalyst for enhancing automobile exhaust purification and preparation method thereof |
| CN113231079B (en) * | 2021-05-26 | 2023-05-02 | 无锡威孚环保催化剂有限公司 | Ternary catalyst for enhancing automobile tail gas purification and preparation method thereof |
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