CN103157470A - Three-element catalyst for automobile exhaust - Google Patents
Three-element catalyst for automobile exhaust Download PDFInfo
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- CN103157470A CN103157470A CN2013100850410A CN201310085041A CN103157470A CN 103157470 A CN103157470 A CN 103157470A CN 2013100850410 A CN2013100850410 A CN 2013100850410A CN 201310085041 A CN201310085041 A CN 201310085041A CN 103157470 A CN103157470 A CN 103157470A
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- cerium zirconium
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- zirconium sosoloid
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Abstract
The invention relates to a three-element catalyst for automobile exhaust. The three-element catalyst for automobile exhaust is characterized by comprising a cellular carrier, wherein a Pd coating is attached to the cellular carrier; an Rh coating is attached to the Pd coating; Rh in the Rh coating is loaded on a zirconium oxide composite oxide and a cerium zirconium solid solution; the zirconium oxide composite oxide is one or more of 80-90wt% of ZrO2, 10-20wt% of La2O3, Y2O3, Pr6O11 and Nd2O3; the cerium zirconium solid solution is one or more of 20-70wt% of ZrO2, 20-70wt% of CeO2, 10-15wt% of La2O3, Y2O3, Pr6O11 and Nd2O3; and the ratio of Rh loaded in the zirconium oxide composite oxide to the cerium zirconium solid solution is (1:1)-(5:1). By using the three-element catalyst, the oxygen storage capability of the catalyst, the high activity of Rh catalytic reduction nitrogen oxide and the high temperature aging resistance of Rh are ensured.
Description
Technical field
The present invention relates to a kind of ternary catalyst for automobile tail gas, belong to the purifying vehicle exhaust technical field.
Background technology
The major pollutants of vehicle exhaust are carbon monoxide (CO), and hydrocarbon (HC) and oxynitrides (NOx) utilize the catalyst that is arranged on 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 comprised 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 being 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 is by the oxygen in adsorption storage tail gas or discharge the ratio that oxygen is regulated oxidisability component and reproducibility component in tail gas, when making carbon monoxide and hydrocarbon oxygen oxidized, oxynitrides is reduced.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 the high temperature of 900 ℃ ~ 1100 ℃.
Mainly make catalyst activity reduction for the alloying action that suppresses Rh and Pd under hot conditions, present three-way catalyst all adopts two coating structures usually, namely be attached to the lower coating loading Pd on honeycomb substrate, and the upper coating that is attached on lower coating supports Rh, in order to make catalyst that enough oxygen storage capacities be arranged, usually in the Rh coating, a large amount of hydrogen-storing materials and a certain amount of aluminium oxide are arranged.Although Rh loads on, oxygen storage capacity is significantly improved, but, the oxygen function of storing of hydrogen-storing material makes the Rh of its load more easily be in oxidation state, 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.And Rh loads on aluminium oxide, can irreversible interaction occur and make the Rh inactivation with aluminium oxide under hot conditions.For this reason, there are in recent years some researchers to propose Rh is loaded on not contain CeO
2Or contain small amount CeO
2ZrO
2Composite oxides on, significantly improved the activity of Rh catalytic reduction oxynitrides after the high temperature ageing, but due to the deficiency of oxygen storage capacity, the pollutant emission of transient condition is very high, especially the tail gas air-fuel ratio is changed highstrung oxynitride discharge.Although can improve oxygen storage capacity by increasing hydrogen-storing material in the Pd of lower floor coating, because gas diffusion length is very large on the impact of oxygen storage capacity, the raising of oxygen storage capacity is very limited.In addition, Pd coating hydrogen-storing material too much also can cause under high-temperature oxygen-enriched condition more Rh to occur to interact and make catalyst activity reduction to lower floor's migration and with Pd.
Summary of the invention
The objective of the invention is to overcome the deficiencies in the prior art, a kind of ternary catalyst for automobile tail gas is provided, have higher carbon monoxide, hydrocarbon and oxynitrides disposal ability have especially improved the activity of Rh catalytic reduction oxynitrides.
According to technical scheme provided by the invention, described ternary catalyst for automobile tail gas comprises honeycomb support, it is characterized in that: adhere to the Pd coating on described honeycomb support, adhere to the Rh coating on the Pd coating; Rh in described Rh coating loads on zirconia composite oxides and cerium zirconium sosoloid, and the component of described zirconia composite oxides is: the ZrO of 80wt% ~ 90wt%
2And the La of 10wt% ~ 20wt%
2O
3, Y
2O
3, Pr
6O
11, Nd
2O
3In one or more, 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; And in described zirconia composite oxides and cerium zirconium sosoloid, the mass ratio of the Rh of load is 1 ~ 5:1.
In a specific embodiment, described Rh coating comprises the zirconia composite oxides of load Rh, cerium zirconium sosoloid and the binding agent of load Rh; Wherein, the zirconia composite oxides of load Rh account for the 30wt% ~ 70wt% of Rh coating quality, and the cerium zirconium sosoloid of load Rh accounts for the 30wt% ~ 70wt% of Rh coating quality, and binding agent accounts for the 3wt% ~ 10wt% of Rh coating quality.
In a specific embodiment, described binding agent is aluminium oxide.
In a specific embodiment, on described honeycomb substrate, the coated weight of Rh coating is 50 ~ 160g/L, and the coated weight of Pd coating is 50 ~ 160g/L.
In a specific embodiment, in described Rh coating, the content of the Rh of load is 0.1 ~ 10g/ft
3
In a specific embodiment, described Pd coating comprises cerium zirconium sosoloid and the La of load P d
2O
3Aluminium oxide (the La of doping
2O
3-Al
2O
3); The cerium zirconium sosoloid of load P d and La
2O
3-Al
2O
3Mass ratio be 1:0.5 ~ 2.
In a specific embodiment, the Pd in described Pd coating loads on cerium zirconium sosoloid, and the component of cerium zirconium sosoloid is: 20wt% ~ 70wt%CeO
2, 20wt% ~ 70wt%ZrO
2And the La of 10wt% ~ 15wt%
2O
3, Y
2O
3, Pr
6O
11, Nd
2O
3In one or more.
In a specific embodiment, at the La of described Pd coating
2O
3-Al
2O
3In, La
2O
3Content account for La-Al
2O
32wt% ~ 10wt%.
In a specific embodiment, in described Pd coating, the content of the Pd of load is 5 ~ 200g/ft
3
Advantage of the present invention is: the coating of three-way catalyst of the present invention is the two coating structures of Pd/Rh, and Rh is loaded on respectively a kind of CeO that do not contain
2The zirconia composite oxides and a kind of cerium zirconium sosoloid on, the ratio that Rh loads on this bi-material is 1:1 ~ 5:1, this design has guaranteed again the high activity of Rh catalytic reduction oxynitrides and the high-temperature aging resisting ability of Rh in the oxygen storage capacity that has guaranteed catalyst; Compare with the two coating three-way catalysts of traditional Pd/Rh, this three-way catalyst disclosed by the invention has high carbon monoxide, and the disposal ability of hydrocarbon and oxynitrides especially has very high oxynitrides conversion capability.
The specific embodiment
The invention will be further described below in conjunction with specific embodiment.
In the Rh coating of three-way catalyst of the present invention, Rh loads on and does not contain CeO
2The zirconia composite oxides and cerium zirconium sosoloid on; Wherein, do not contain CeO
2The consisting of of zirconia composite oxides: the ZrO of 80wt% ~ 90wt%
2And the La of 10wt% ~ 20wt%
2O
3, Y
2O
3, Pr
6O
11, Nd
2O
3In one or more, La
2O
3, Y
2O
3, Pr
6O
11, Nd
2O
3In order to improve ZrO
2Heat endurance.
In described Rh coating, the cerium zirconium sosoloid of load Rh consists of: 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, La
2O
3, Y
2O
3, Pr6O
11, Nd
2O
3In order to improve the heat endurance of cerium zirconium sosoloid.
Embodiment one: a kind of ternary catalyst for automobile tail gas, comprise cellular structure ceramic carrier, and specification is Ф 118.4mm * 152.4mm, and hole density is 600cpsi, and the duct wall thickness is 4.3mil, and volume is 1.678L; Adhere to the Pd coating on honeycomb support, the coated weight of Pd coating is 120g/L, adheres to the Rh coating on the Pd coating, and the coated weight of Rh coating is 120g/L; Wherein, the Pd in the Pd coating loads on cerium zirconium sosoloid, and the content of Pd is 27g/ft
3Rh in the Rh coating loads on zirconia composite oxides and cerium zirconium sosoloid, and Rh content is 3g/ ft
3
The coating procedure of described Pd coating is: with the cerium zirconium sosoloid of the load P d of 1000g, the La of 1000g
2O
3-Al
2O
3Mix with appropriate amount of deionized water, obtain the coating slurries after ball milling; These coating slurries are coated on cellular structure ceramic carrier, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtain the Pd coating; Wherein, the component of cerium zirconium sosoloid is: 45wt%CeO
2, 45wt%ZrO
2, 5wt% La
2O
3And 5wt%Pr
6O
11At La
2O
3-Al
2O
3In, La
2O
3Content account for La-Al
2O
34wt%;
The coating procedure of described Rh coating is: the cerium zirconium sosoloid of 475g load Rh, zirconia composite oxides, 50g aluminium oxide and appropriate amount of deionized water with 475g load Rh are mixed (wherein, in zirconia composite oxides and cerium zirconium sosoloid, the ratio of the Rh of load is 2:1), obtain the coating slurries after ball milling; On ceramic monolith after these coating slurries are coated to the Pd coating and apply, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtain the Rh coating; Wherein, the component of zirconia composite oxides is: the ZrO of 85wt%
2, 5wt% La
2O
3, 5wt% Y
2O
3And 5wt%, the component of described cerium zirconium sosoloid is: 45% ZrO
2, 45wt% CeO
2, 5wt% La
2O
3, 5wt% Nd
2O
3
Embodiment two: a kind of ternary catalyst for automobile tail gas, comprise cellular structure ceramic carrier, and specification is Ф 118.4mm * 152.4mm, and hole density is 600cpsi, and the duct wall thickness is 4.3mil, and volume is 1.678L; Adhere to the Pd coating on honeycomb support, the coated weight of Pd coating is 120g/L, adheres to the Rh coating on the Pd coating, and the coated weight of Rh coating is 120g/L; Wherein, the Pd in the Pd coating loads on cerium zirconium sosoloid, and the content of Pd is 27g/ft
3Rh in the Rh coating loads on zirconia composite oxides and cerium zirconium sosoloid, and Rh content is 3g/ft
3
The coating procedure of described Pd coating is: with the cerium zirconium sosoloid of the load P d of 1000g, the La of 1000g
2O
3-Al
2O
3Mix with appropriate amount of deionized water, obtain the coating slurries after ball milling; These coating slurries are coated on cellular structure ceramic carrier, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtain the Pd coating; Wherein, the component of cerium zirconium sosoloid is: 45wt%CeO
2, 45wt%ZrO
2, 5wt% La
2O
3And 5wt%Pr
6O
11At La
2O
3-Al
2O
3In, La
2O
3Content account for La-Al
2O
34wt%;
The coating procedure of described Rh coating is: the cerium zirconium sosoloid of 475g load Rh, zirconia composite oxides, 50g aluminium oxide and appropriate amount of deionized water with 475g load Rh are mixed (wherein, in zirconia composite oxides and cerium zirconium sosoloid, the ratio of the Rh of load is 4:1), obtain the coating slurries after ball milling; On ceramic monolith after these coating slurries are coated to the Pd coating and apply, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtain the Rh coating; Wherein, the component of zirconia composite oxides is: the ZrO of 85wt%
2, 5wt% La
2O
3, 5wt% Y
2O
3And 5wt%, the component of described cerium zirconium sosoloid is: the ZrO of 45wt%
2, 45wt% CeO
2, 5wt% La
2O
3, 5wt% Nd
2O
3
Embodiment three: a kind of ternary catalyst for automobile tail gas, comprise cellular structure ceramic carrier, and specification is Ф 118.4mm * 152.4mm, and hole density is 600cpsi, and the duct wall thickness is 4.3mil, and volume is 1.678L; Adhere to the Pd coating on honeycomb support, the coated weight of Pd coating is 50g/L, adheres to the Rh coating on the Pd coating, and the coated weight of Rh coating is 50g/L; Wherein, the Pd in the Pd coating loads on cerium zirconium sosoloid, and the content of Pd is 5g/ft
3Rh in the Rh coating loads on zirconia composite oxides and cerium zirconium sosoloid, and Rh content is 0.1g/ft
3
The coating procedure of described Pd coating is: with the cerium zirconium sosoloid of the load P d of 1000g, the La of 500g
2O
3-Al
2O
3Mix with appropriate amount of deionized water, obtain the coating slurries after ball milling; These coating slurries are coated on cellular structure ceramic carrier, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtain the Pd coating; Wherein, the component of cerium zirconium sosoloid is: 20wt%CeO
2, 70wt%ZrO
2La with 5wt%
2O
3Y with 5wt%
2O
3At La
2O
3-Al
2O
3In, La
2O
3Content account for La-Al
2O
32wt%;
The coating procedure of described Rh coating is: the cerium zirconium sosoloid of 475g load Rh, zirconia composite oxides, 47.5g aluminium oxide and appropriate amount of deionized water with 475g load Rh are mixed (wherein, in zirconia composite oxides and cerium zirconium sosoloid, the ratio of the Rh of load is 1:1), obtain the coating slurries after ball milling; On ceramic monolith after these coating slurries are coated to the Pd coating and apply, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtain the Rh coating; Wherein, the component of zirconia composite oxides is: the ZrO of 80wt%
2, 5wt% La
2O
3, 5wt% Y
2O
3, 5wt% Pr
6O
11Nd with 5wt%
2O
3, the component of described cerium zirconium sosoloid is: the ZrO of 20wt%
2, 70wt% CeO
2, 5wt% La
2O
3Y with 5wt%
2O
3
Embodiment four: a kind of ternary catalyst for automobile tail gas, comprise cellular structure ceramic carrier, and specification is Ф 118.4mm * 152.4mm, and hole density is 600cpsi, and the duct wall thickness is 4.3mil, and volume is 1.678L; Adhere to the Pd coating on honeycomb support, the coated weight of Pd coating is 160g/L, adheres to the Rh coating on the Pd coating, and the coated weight of Rh coating is 160g/L; Wherein, the Pd in the Pd coating loads on cerium zirconium sosoloid, and the content of Pd is 200g/ft
3Rh in the Rh coating loads on zirconia composite oxides and cerium zirconium sosoloid, and Rh content is 10g/ft
3
The coating procedure of described Pd coating is: with the cerium zirconium sosoloid of the load P d of 500g, the La of 1000g
2O
3-Al
2O
3Mix with appropriate amount of deionized water, obtain the coating slurries after ball milling; These coating slurries are coated on cellular structure ceramic carrier, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtain the Pd coating; Wherein, the component of cerium zirconium sosoloid is: 70wt%CeO
2, 20%ZrO
2, 5wt% La
2O
3With 5wt%'s; At La
2O
3-Al
2O
3In, La
2O
3Content account for La-Al
2O
310wt%;
The coating procedure of described Rh coating is: the cerium zirconium sosoloid of 475g load Rh, zirconia composite oxides, 50g aluminium oxide and appropriate amount of deionized water with 475g load Rh are mixed (wherein, in zirconia composite oxides and cerium zirconium sosoloid, the ratio of the Rh of load is 1:1), obtain the coating slurries after ball milling; On ceramic monolith after these coating slurries are coated to the Pd coating and apply, and 450 ℃ ~ 600 ℃ roasting temperatures 1 ~ 5 hour, obtain the Rh coating; Wherein, the component of zirconia composite oxides is: the ZrO of 90wt%
2, 5wt% La
2O
3Y with 5wt%
2O
3, the component of described 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, do not contain CeO except Rh loads on
2The zirconia composite oxides and the ratio on cerium zirconium sosoloid become 1:2.
Comparative Examples 2: each parameter, composition and preparation process are identical with embodiment 1, will not contain CeO
2The zirconia composite oxides by La
2O
3The aluminium oxide of doping replaces, wherein La
2O
3At La
2O
3Account for 4wt% in the aluminium oxide of doping.
With embodiment 1, embodiment 2 and Comparative Examples 1, the resulting catalyst sample of Comparative Examples 2 all according to the aging circulation of GMAC875 stand of General Motors Overseas Corporation with condition after aging 50 hours, the car load emission test loops by ECE+EUDC, the engine displacement 1.8L of testing vehicle.The emission test result is as shown in table 1.
Table 1
| ? | Hydrocarbon (g/km) | Carbon monoxide (g/km) | Oxynitrides (g/km) |
| Embodiment 1 | 0.0522 | 0.723 | 0.0432 |
| Embodiment 2 | 0.0373 | 0.783 | 0.0552 |
| Comparative Examples 1 | 0.0501 | 0.700 | 0.0784 |
| Comparative Examples 2 | 0.0566 | 0.932 | 0.0886 |
As shown in table 1, the result of catalyst performance evaluation shows, compares with Comparative Examples 1,2, and the embodiment of the present invention 1,2 disclosed three-way catalysts have higher pollutant disposal ability, especially more excellent oxynitrides conversion capability.
Claims (9)
1. a ternary catalyst for automobile tail gas, comprise honeycomb support, it is characterized in that: adhere to the Pd coating on described honeycomb support, adhere to the Rh coating on the Pd coating; Rh in described Rh coating loads on zirconia composite oxides and cerium zirconium sosoloid, and the component of described zirconia composite oxides is: the ZrO of 80wt% ~ 90wt%
2And the La of 10wt% ~ 20wt%
2O
3, Y
2O
3, Pr
6O
11, Nd
2O
3In one or more, the component of described cerium zirconium sosoloid is: the ZrO of 20wt% ~ 70%wt
2, 20wt% ~ 70wt% CeO
2And the La of 10wt% ~ 15wt%
2O
3, Y
2O
3, Pr6O
11, Nd
2O
3In one or more; And in described zirconia composite oxides and cerium zirconium sosoloid, the mass ratio of the Rh of load is 1 ~ 5:1.
2. ternary catalyst for automobile tail gas as claimed in claim 1, it is characterized in that: described Rh coating comprises the zirconia composite oxides of load Rh, cerium zirconium sosoloid and the binding agent of load Rh; Wherein, the zirconia composite oxides of load Rh account for the 30wt% ~ 70wt% of Rh coating quality, and the cerium zirconium sosoloid of load Rh accounts for the 30wt% ~ 70wt% of Rh coating quality, and binding agent accounts for the 3wt% ~ 10wt% of Rh coating quality.
3. ternary catalyst for automobile tail gas as claimed in claim 2, it is characterized in that: described binding agent is aluminium oxide.
4. ternary catalyst for automobile tail gas as claimed in claim 1, it is characterized in that: on described honeycomb substrate, the coated weight of Rh coating is 50 ~ 160g/L, and the coated weight of Pd coating is 50 ~ 160g/L.
5. ternary catalyst for automobile tail gas as claimed in claim 1, it is characterized in that: in described Rh coating, the content of the Rh of load is 0.1 ~ 10g/ft
3
6. ternary catalyst for automobile tail gas as claimed in claim 1, it is characterized in that: described Pd coating comprises cerium zirconium sosoloid and the La of load P d
2O
3Aluminium oxide (the La of doping
2O
3-Al
2O
3); The cerium zirconium sosoloid of load P d and La
2O
3-Al
2O
3Mass ratio be 1:0.5 ~ 2.
7. ternary catalyst for automobile tail gas as claimed in claim 6, it is characterized in that: the Pd in described Pd coating loads on cerium zirconium sosoloid, and the component of cerium zirconium sosoloid is: 20wt ~ 70wt%CeO
2, 20wt ~ 70wt%ZrO
2And the La of 10wt% ~ 15wt%
2O
3, Y
2O
3, Pr
6O
11, Nd
2O
3In one or more.
8. ternary catalyst for automobile tail gas as claimed in claim 6, is characterized in that: at the La of described Pd coating
2O
3-Al
2O
3In, La
2O
3Content account for La-Al
2O
32wt% ~ 10wt%.
9. ternary catalyst for automobile tail gas as claimed in claim 6, it is characterized in that: in described Pd coating, the content of the Pd of load is 5 ~ 200g/ft
3
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| CN104148068A (en) * | 2014-08-06 | 2014-11-19 | 无锡威孚环保催化剂有限公司 | Three-way catalyst capable of quickly igniting automobile exhaust |
| CN104785257A (en) * | 2015-04-02 | 2015-07-22 | 无锡威孚环保催化剂有限公司 | Single-coating three-way catalyst and preparation method thereof |
| CN105597748A (en) * | 2015-11-13 | 2016-05-25 | 无锡威孚环保催化剂有限公司 | Segmented type ternary catalyst and preparation method thereof |
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| CN112023986A (en) * | 2020-09-18 | 2020-12-04 | 无锡威孚环保催化剂有限公司 | Automobile exhaust purification catalyst and preparation method thereof |
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