CN103157470B - Ternary catalyst for automobile tail gas - Google Patents
Ternary catalyst for automobile tail gas Download PDFInfo
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- CN103157470B CN103157470B CN201310085041.0A CN201310085041A CN103157470B CN 103157470 B CN103157470 B CN 103157470B CN 201310085041 A CN201310085041 A CN 201310085041A CN 103157470 B CN103157470 B CN 103157470B
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Abstract
The present invention relates to a kind of ternary catalyst for automobile tail gas, it is characterized in that: comprise honeycomb support, honeycomb support adheres to Pd coating, Pd coating is adhered to Rh coating; Rh load in described Rh coating is on zirconia composite oxide and cerium zirconium sosoloid, and the component of described zirconia composite oxide is: the ZrO of 80wt% ~ 90wt%
2with 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%
2, 20wt% ~ 70wt% CeO
2with the La of 10wt% ~ 15wt%
2o
3, Y
2o
3, Pr6O
11, Nd
2o
3in one or more; And the ratio of the Rh of load is 1:1 ~ 5:1 in described zirconia composite oxide and cerium zirconium sosoloid.Three-way catalyst of the present invention, while ensure that the oxygen storage capacity of catalyst, in turn ensure that the high activity of Rh catalytic reduction oxynitrides and the high-temperature aging resisting ability of Rh.
Description
Technical field
The present invention relates to a kind of ternary catalyst for automobile tail gas, belong to 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 being arranged on gas extraction system carbon monoxide, oxidizing hydrocarbon can be become carbon dioxide (CO
2), water (H
2and make oxynitrides be reduced to nitrogen (N O), simultaneously
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 is attached to supported catalyst coating.Catalyst coat is usually by having compared with the oxide material (as aluminium oxide) of bigger serface, hydrogen-storing material and the noble metal active component (normal is Pt(platinum), the Pd(palladium that are dispersed in oxide or hydrogen-storing material surface), Rh(rhodium) in one or more) form.Hydrogen-storing material is wherein generally the composite oxides containing cerium zirconium, it is by the oxygen in adsorption storage tail gas or discharge the ratio that oxygen regulates oxidizing component and reproducibility component in tail gas, make carbon monoxide and hydrocarbon oxygen oxidized while, oxynitrides is reduced.The transformation efficiency of pollutant during in order to improve cold-starting automobile, three-way catalyst is often installed in the position near enmgine exhaust outlet, and when galloping, the bed temperature of three-way catalyst can reach the high temperature of 900 DEG C ~ 1100 DEG C.
Catalyst activity reduction is made mainly for the alloying action of Rh and Pd under suppression hot conditions, current three-way catalyst all adopts two coating structure usually, namely the lower coating loading Pd on honeycomb substrate is attached to, and the upper coating be attached in lower coating supports Rh, in order to make catalyst have enough oxygen storage capacities, usually there are a large amount of hydrogen-storing materials and a certain amount of aluminium oxide in Rh coating.Although Rh load can make oxygen storage capacity significantly improve on hydrogen-storing material, 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 thickened.And Rh load on alumina, can irreversible interaction be there is with aluminium oxide and make Rh inactivation under the high temperature conditions.For this reason, some researchers are had to propose Rh load not containing CeO in recent years
2or containing small amount CeO
2zrO
2composite oxides on, significantly improve the activity of Rh catalytic reduction oxynitrides after high temperature ageing, but due to the deficiency of oxygen storage capacity, the pollutant emission of transient condition is very high, especially changes highstrung oxynitride discharge to tail gas air-fuel ratio.Although improve oxygen storage capacity by increasing hydrogen-storing material in lower floor Pd 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 to cause under high-temperature oxygen-enriched condition more Rh to lower floor's migration and occur to interact with Pd and make catalyst activity reduction.
Summary of the invention
The object of the invention is to overcome the deficiencies in the prior art, provide a kind of ternary catalyst for automobile tail gas, have higher carbon monoxide, hydrocarbon and oxynitrides disposal ability, especially improve 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: on described honeycomb support, adhere to Pd coating, and Pd coating is adhered to Rh coating; Rh load in described Rh coating is on zirconia composite oxide and cerium zirconium sosoloid, and the component of described zirconia composite oxide is: the ZrO of 80wt% ~ 90wt%
2with 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
2with the La of 10wt% ~ 15wt%
2o
3, Y
2o
3, Pr6O
11, Nd
2o
3in one or more; And the mass ratio of the Rh of load is 1 ~ 5:1 in described zirconia composite oxide and cerium zirconium sosoloid.
In a detailed description of the invention, described Rh coating comprises the zirconia composite oxide of load Rh, the cerium zirconium sosoloid of load Rh and binding agent; Wherein, the zirconia composite oxide of load Rh accounts 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 detailed description of the invention, described binding agent is aluminium oxide.
In a detailed description of the invention, on described honeycomb substrate, the coated weight of Rh coating is the coated weight of 50 ~ 160g/L, Pd coating is 50 ~ 160g/L.
In a detailed description of the invention, in described Rh coating, the content of the Rh of load is 0.1 ~ 10g/ft
3.
In a detailed description of the invention, 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 detailed description of the invention, the Pd load in described Pd coating is on cerium zirconium sosoloid, and the component of cerium zirconium sosoloid is: 20wt% ~ 70wt%CeO
2, 20wt% ~ 70wt%ZrO
2with the La of 10wt% ~ 15wt%
2o
3, Y
2o
3, Pr
6o
11, Nd
2o
3in one or more.
In a detailed description of the invention, at the La of described Pd coating
2o
3-Al
2o
3in, La
2o
3content account for La-Al
2o
32wt% ~ 10wt%.
In a detailed description of the invention, 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 structure of Pd/Rh, and the load of Rh difference is not contained CeO in one
2zirconia composite oxide and a kind of cerium zirconium sosoloid on, the ratio of Rh load on this bi-material is 1:1 ~ 5:1, this design, while ensure that the oxygen storage capacity of catalyst, in turn ensure that the high activity of Rh catalytic reduction oxynitrides and the high-temperature aging resisting ability of Rh; Compared with the two coating three-way catalyst of traditional Pd/Rh, this three-way catalyst disclosed by the invention has high carbon monoxide, the disposal ability of hydrocarbon and oxynitrides, especially has very high oxynitrides conversion capability.
Detailed description of the invention
Below in conjunction with specific embodiment, the invention will be further described.
In the Rh coating of three-way catalyst of the present invention, Rh load is not containing CeO
2zirconia composite oxide and cerium zirconium sosoloid on; Wherein, not containing CeO
2the consisting of of zirconia composite oxide: the ZrO of 80wt% ~ 90wt%
2with 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
2with 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, comprises cellular structure ceramic carrier, specification is Ф 118.4mm × 152.4mm, and hole density is 600cpsi, and duct wall thickness is 4.3mil, and volume is 1.678L; Honeycomb support adheres to Pd coating, and the coated weight of Pd coating is 120g/L, and Pd coating is adhered to Rh coating, and the coated weight of Rh coating is 120g/L; Wherein, the Pd load in Pd coating is on cerium zirconium sosoloid, and the content of Pd is 27g/ft
3; Rh load in Rh coating is on zirconia composite oxide and cerium zirconium sosoloid, and Rh content is 3g/ ft
3;
The coating procedure of described Pd coating is: by the cerium zirconium sosoloid of the load P d of 1000g, the La of 1000g
2o
3-Al
2o
3with appropriate amount of deionized water mixing, after ball milling, obtain coating slurry; This coating slurry is coated on cellular structure ceramic carrier, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains Pd coating; Wherein, the component of cerium zirconium sosoloid is: 45wt%CeO
2, 45wt%ZrO
2, 5wt% La
2o
3and 5wt%Pr
6o
11; At La
2o
3-Al
2o
3in, La
2o
3content account for La-Al
2o
34wt%;
The coating procedure of described Rh coating is: mix (wherein by the cerium zirconium sosoloid of 475g load Rh, zirconia composite oxide, 50g aluminium oxide and appropriate amount of deionized water with 475g load Rh, in zirconia composite oxide and cerium zirconium sosoloid, the ratio of the Rh of load is 2:1), after ball milling, obtain coating slurry; This coating slurry is coated on the ceramic monolith after the coating of Pd coating, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains Rh coating; Wherein, the component of zirconia composite oxide 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 45%
2, 45wt% CeO
2, 5wt% La
2o
3, 5wt% Nd
2o
3.
Embodiment two: a kind of ternary catalyst for automobile tail gas, comprises cellular structure ceramic carrier, specification is Ф 118.4mm × 152.4mm, and hole density is 600cpsi, and duct wall thickness is 4.3mil, and volume is 1.678L; Honeycomb support adheres to Pd coating, and the coated weight of Pd coating is 120g/L, and Pd coating is adhered to Rh coating, and the coated weight of Rh coating is 120g/L; Wherein, the Pd load in Pd coating is on cerium zirconium sosoloid, and the content of Pd is 27g/ft
3; Rh load in Rh coating is on zirconia composite oxide and cerium zirconium sosoloid, and Rh content is 3g/ft
3;
The coating procedure of described Pd coating is: by the cerium zirconium sosoloid of the load P d of 1000g, the La of 1000g
2o
3-Al
2o
3with appropriate amount of deionized water mixing, after ball milling, obtain coating slurry; This coating slurry is coated on cellular structure ceramic carrier, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains Pd coating; Wherein, the component of cerium zirconium sosoloid is: 45wt%CeO
2, 45wt%ZrO
2, 5wt% La
2o
3and 5wt%Pr
6o
11; At La
2o
3-Al
2o
3in, La
2o
3content account for La-Al
2o
34wt%;
The coating procedure of described Rh coating is: mix (wherein by the cerium zirconium sosoloid of 475g load Rh, zirconia composite oxide, 50g aluminium oxide and appropriate amount of deionized water with 475g load Rh, in zirconia composite oxide and cerium zirconium sosoloid, the ratio of the Rh of load is 4:1), after ball milling, obtain coating slurry; This coating slurry is coated on the ceramic monolith after the coating of Pd coating, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains Rh coating; Wherein, the component of zirconia composite oxide 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, comprises cellular structure ceramic carrier, specification is Ф 118.4mm × 152.4mm, and hole density is 600cpsi, and duct wall thickness is 4.3mil, and volume is 1.678L; Honeycomb support adheres to Pd coating, and the coated weight of Pd coating is 50g/L, and Pd coating is adhered to Rh coating, and the coated weight of Rh coating is 50g/L; Wherein, the Pd load in Pd coating is on cerium zirconium sosoloid, and the content of Pd is 5g/ft
3; Rh load in Rh coating is on zirconia composite oxide and cerium zirconium sosoloid, and Rh content is 0.1g/ft
3;
The coating procedure of described Pd coating is: by the cerium zirconium sosoloid of the load P d of 1000g, the La of 500g
2o
3-Al
2o
3with appropriate amount of deionized water mixing, after ball milling, obtain coating slurry; This coating slurry is coated on cellular structure ceramic carrier, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains Pd coating; Wherein, the component of cerium zirconium sosoloid is: 20wt%CeO
2, 70wt%ZrO
2with the La of 5wt%
2o
3with the Y of 5wt%
2o
3; At La
2o
3-Al
2o
3in, La
2o
3content account for La-Al
2o
32wt%;
The coating procedure of described Rh coating is: mix (wherein by the cerium zirconium sosoloid of 475g load Rh, zirconia composite oxide, 47.5g aluminium oxide and appropriate amount of deionized water with 475g load Rh, in zirconia composite oxide and cerium zirconium sosoloid, the ratio of the Rh of load is 1:1), after ball milling, obtain coating slurry; This coating slurry is coated on the ceramic monolith after the coating of Pd coating, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains Rh coating; Wherein, the component of zirconia composite oxide is: the ZrO of 80wt%
2, 5wt% La
2o
3, 5wt% Y
2o
3, 5wt% Pr
6o
11with the Nd of 5wt%
2o
3, the component of described cerium zirconium sosoloid is: the ZrO of 20wt%
2, 70wt% CeO
2, 5wt% La
2o
3with the Y of 5wt%
2o
3.
Embodiment four: a kind of ternary catalyst for automobile tail gas, comprises cellular structure ceramic carrier, specification is Ф 118.4mm × 152.4mm, and hole density is 600cpsi, and duct wall thickness is 4.3mil, and volume is 1.678L; Honeycomb support adheres to Pd coating, and the coated weight of Pd coating is 160g/L, and Pd coating is adhered to Rh coating, and the coated weight of Rh coating is 160g/L; Wherein, the Pd load in Pd coating is on cerium zirconium sosoloid, and the content of Pd is 200g/ft
3; Rh load in Rh coating is on zirconia composite oxide and cerium zirconium sosoloid, and Rh content is 10g/ft
3;
The coating procedure of described Pd coating is: by the cerium zirconium sosoloid of the load P d of 500g, the La of 1000g
2o
3-Al
2o
3with appropriate amount of deionized water mixing, after ball milling, obtain coating slurry; This coating slurry is coated on cellular structure ceramic carrier, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains 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: mix (wherein by the cerium zirconium sosoloid of 475g load Rh, zirconia composite oxide, 50g aluminium oxide and appropriate amount of deionized water with 475g load Rh, in zirconia composite oxide and cerium zirconium sosoloid, the ratio of the Rh of load is 1:1), after ball milling, obtain coating slurry; This coating slurry is coated on the ceramic monolith after the coating of Pd coating, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains Rh coating; Wherein, the component of zirconia composite oxide is: the ZrO of 90wt%
2, 5wt% La
2o
3with the Y of 5wt%
2o
3, the component of described cerium zirconium sosoloid is: the ZrO of 70wt%
2, 20wt% CeO
2, 5wt% La
2o
3with the Y of 5wt%
2o
3.
Comparative example 1: each parameter, composition are identical with embodiment 1 with preparation process, except Rh load is not containing CeO
2zirconia composite oxide and cerium zirconium sosoloid on ratio become 1:2.
Comparative example 2: each parameter, composition are identical with embodiment 1 with preparation process, will not contain CeO
2zirconia composite oxide by La
2o
3the aluminium oxide of doping replaces, wherein La
2o
3at La
2o
34wt% is accounted in the aluminium oxide of doping.
The catalyst sample that embodiment 1, embodiment 2 and comparative example 1, comparative example 2 are obtained all according to the GMAC875 stand ageing cycle of General Motors Overseas Corporation with condition after aging 50 hours, car load emission test is undertaken by ECE+EUDC circulation, the engine displacement 1.8L of testing vehicle.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 example 1 | 0.0501 | 0.700 | 0.0784 |
| Comparative example 2 | 0.0566 | 0.932 | 0.0886 |
As shown in table 1, the result of catalyst performance evaluation shows, compared with comparative example 1,2, the three-way catalyst disclosed in the embodiment of the present invention 1,2 has higher pollutant disposal ability, especially more excellent oxynitrides conversion capability.
Claims (7)
1. a ternary catalyst for automobile tail gas, comprises honeycomb support, it is characterized in that: on described honeycomb support, adhere to Pd coating, and Pd coating is adhered to Rh coating; Rh load in described Rh coating is on zirconia composite oxide and cerium zirconium sosoloid, and the component of zirconia composite oxide is: the ZrO of 80wt%
2, 5wt% La
2o
3, 5wt% Y
2o
3, 5wt% Pr
6o
11with the Nd of 5wt%
2o
3, the component of described cerium zirconium sosoloid is: the ZrO of 20wt%
2, 70wt% CeO
2, 5wt% La
2o
3with the Y of 5wt%
2o
3; And the mass ratio of the Rh of load is 1:1 in described zirconia composite oxide and cerium zirconium sosoloid;
The coating procedure of described Rh coating is: the cerium zirconium sosoloid of 475g load Rh, zirconia composite oxide, 47.5g aluminium oxide and appropriate amount of deionized water with 475g load Rh are mixed, after ball milling, obtain coating slurry; This coating slurry is coated on the ceramic monolith after the coating of Pd coating, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains Rh coating.
2. ternary catalyst for automobile tail gas as claimed in claim 1, is characterized in that: on described honeycomb substrate, and the coated weight of Rh coating is the coated weight of 50 ~ 160g/L, Pd coating is 50 ~ 160g/L.
3. ternary catalyst for automobile tail gas as claimed in claim 1, is characterized in that: in described Rh coating, the content of the Rh of load is 0.1 ~ 10g/ft
3.
4. ternary catalyst for automobile tail gas as claimed in claim 1, 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.
5. ternary catalyst for automobile tail gas as claimed in claim 4, is characterized in that: the Pd load in described Pd coating is on cerium zirconium sosoloid, and the component of cerium zirconium sosoloid is: 20wt ~ 70wt%CeO
2, 20wt ~ 70wt%ZrO
2with the La of 10wt% ~ 15wt%
2o
3, Y
2o
3, Pr
6o
11, Nd
2o
3in one or more.
6. ternary catalyst for automobile tail gas as claimed in claim 4, is characterized in that: at the La of described Pd coating
2o
3-Al
2o
3in, La
2o
3content account for La
2o
3-Al
2o
32wt% ~ 10wt%.
7. ternary catalyst for automobile tail gas as claimed in claim 4, is characterized in that: in described Pd coating, the content of the Pd of load is 5 ~ 200g/ft
3.
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| CN101495233A (en) * | 2006-07-25 | 2009-07-29 | 丰田自动车株式会社 | Catalyst for exhaust gas purification |
| CN1935368A (en) * | 2006-09-06 | 2007-03-28 | 天津化工研究设计院 | Method for preparing purifying catalyst for reducing cold-start exhaust emission |
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