CN103191734B - Three-element catalyst for treating automobile exhaust - Google Patents
Three-element catalyst for treating automobile exhaust Download PDFInfo
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- CN103191734B CN103191734B CN201310083742.0A CN201310083742A CN103191734B CN 103191734 B CN103191734 B CN 103191734B CN 201310083742 A CN201310083742 A CN 201310083742A CN 103191734 B CN103191734 B CN 103191734B
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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 vehicle maintenance service, 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 oxidized while oxynitrides be 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 be attached to the lower coating loading Pd on honeycomb substrate, coating material generally comprises cerium zirconium sosoloid, aluminium oxide and other auxiliary agents; And the upper coating be attached in lower coating supports Rh, coating material generally also comprises cerium zirconium sosoloid, aluminium oxide and other auxiliary agents.But under high-temperature oxygen-enriched condition, the easy coating downwards of Rh of upper coating is moved and is interacted with Pd, and makes the activity decrease of catalyst.In addition, 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 reduction of oxidation state is very low, even at motor exhaust by rare transient condition thickened.
Summary of the invention
The object of the invention is to overcome the deficiencies in the prior art, a kind of three-way catalyst for vehicle maintenance service is provided, there is higher hydrocarbon, carbon monoxide and oxynitrides disposal ability, it suppresses Rh to the migration of Pd coating, improves the activity of Rh catalytic reduction oxynitrides.
According to technical scheme provided by the invention, the described three-way catalyst for vehicle maintenance service, comprises honeycomb support, it is characterized in that: on described honeycomb support, adhere to lower floor Pd coating, in lower floor Pd coating, Pd coating in the middle of attachment, middle Pd coating is adhered to upper strata Rh coating; Described lower floor 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), 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 detailed description of the invention, in described lower floor Pd coating, the cerium zirconium sosoloid of load P d and La
2o
3-Al
2o
3mass ratio be 1 ~ 3:1.
In a detailed description of the invention, in described middle Pd coating, binding agent accounts for the 1wt% ~ 10wt% of middle Pd coating gross mass.
In a detailed description of the invention, 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 detailed description of the invention, 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.
In a detailed description of the invention, in described lower floor Pd coating, the load capacity of Pd is 5 ~ 200g/ft
3, in middle Pd coating, the load capacity of Pd is 5 ~ 200g/ft
3, in the Rh coating of upper strata, the load capacity of Rh is 0.1 ~ 10g/ft
3.
In a detailed description of the invention, in described lower floor Pd coating and middle Pd coating, the mass ratio of the Pd of load is 3:1 ~ 9.
In a detailed description of the invention, the coated weight of described lower floor Pd 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 detailed description of the invention, described La
2o
3-Al
2o
3in La
2o
3content accounts for La
2o
3-Al
2o
32wt% ~ 10wt%.
In a detailed description of the invention, described binding agent is ZrO
2.
Advantage of the present invention is: (1) three-way catalyst of the present invention is Pd/Pd/Rh tri-coating structure, owing to not containing CeO in middle Pd coating
2component, inhibits upper strata Rh to the migration of middle Pd coating; (2) three-way catalyst of the present invention is not owing to containing CeO in middle Pd coating
2component, and Pd load is at La
2o
3-Al
2o
3on, improve the catalytic capability of catalyst; (3) in the lower floor Pd coating of three-way catalyst of the present invention, Pd is supported on cerium zirconium sosoloid, improves the oxygen storage capacity of catalyst; (4) three-way catalyst of the present invention is compared with the two coating three-way catalyst of traditional Pd/Rh, has higher hydrocarbon, carbon monoxide and oxynitrides disposal ability, especially has higher oxynitrides conversion capability.
Detailed description of the invention
Below in conjunction with specific embodiment, the invention will be further described.
Embodiment 1: a kind of three-way catalyst for vehicle maintenance service, comprises honeycomb support, and specification is Ф 118.4mm × 152.4mm, and Kong Mi counts 600cpsi, duct wall thickness is 4.3mil, and volume is 1.678L; Described honeycomb support adheres to lower floor Pd coating, and in lower floor Pd coating, Pd coating in the middle of attachment, middle Pd coating is adhered to upper strata Rh coating; Described lower floor 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), 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
3; In described lower floor Pd coating, the load capacity of Pd is 18g/ft
3, in middle Pd coating, the load capacity of Pd is 18g/ft
3, in the Rh coating of upper strata, the load capacity of Rh is 4g/ft
3;
The preparation method of described three-way catalyst, adopts following processing step:
The coating procedure of the 1st step, described lower floor Pd coating: by 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 mixing, and after ball milling preparation obtain coating slurry; Be coated on honeycomb support by this coating slurry, the coated weight of lower floor Pd coating is 60g/L, and 450 DEG C ~ 600 DEG C 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
3with the Pr6O of 5wt%
11;
The coating procedure of the 2nd step, described middle Pd coating: by 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%), 400 zirconium oxyacetate solution are (containing the ZrO of 84g
2) and appropriate amount of deionized water mixing, and preparation obtains coating slurry after ball milling; This coating slurry is coated to the 1st step complete after honeycomb support on, the coated weight of middle Pd coating is 60g/L, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains middle Pd coating;
The coating procedure of the 3rd step, described upper strata Rh coating: by 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 mixing, and after ball milling preparation obtain coating slurry; This coating slurry is coated to the 2nd step complete after honeycomb support on, upper strata Rh coating be applied to 100g/L, and 450 DEG C ~ 600 DEG C 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 vehicle maintenance service, comprises honeycomb support, and specification is Ф 118.4mm × 152.4mm, and Kong Mi counts 600cpsi, duct wall thickness is 4.3mil, and volume is 1.678L; Described honeycomb support adheres to lower floor Pd coating, and in lower floor Pd coating, Pd coating in the middle of attachment, middle Pd coating is adhered to upper strata Rh coating; Described lower floor 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), 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
3; In described lower floor Pd coating, the load capacity of Pd is 15g/ft
3, in middle Pd coating, the load capacity of Pd is 5g/ft
3, in the Rh coating of upper strata, the load capacity of Rh is 0.1g/ft
3;
The preparation method of described three-way catalyst, adopts following processing step:
The coating procedure of the 1st step, described lower floor Pd coating: by 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 mixing, and after ball milling preparation obtain coating slurry; Be coated on honeycomb support by this coating slurry, the coated weight of lower floor Pd coating is 30g/L, and 450 DEG C ~ 600 DEG C 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
11with the Nd of 5wt%
2o
3;
The coating procedure of the 2nd step, described middle Pd coating: by 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%), 400 zirconium oxyacetate solution are (containing the ZrO of 84g
2) and appropriate amount of deionized water mixing, and preparation obtains coating slurry after ball milling; This coating slurry is coated to the 1st step complete after honeycomb support on, the coated weight of middle Pd coating is 30g/L, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains middle Pd coating;
The coating procedure of the 3rd step, described upper strata Rh coating: by 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 mixing, and after ball milling preparation obtain coating slurry; This coating slurry is coated to the 2nd step complete after honeycomb support on, upper strata Rh coating be applied to 50 ~ 160g/L, and 450 DEG C ~ 600 DEG C 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
11with the Nd of 5wt%
2o
3.
Embodiment 3: a kind of three-way catalyst for vehicle maintenance service, comprises honeycomb support, and specification is Ф 118.4mm × 152.4mm, and Kong Mi counts 600cpsi, duct wall thickness is 4.3mil, and volume is 1.678L; Described honeycomb support adheres to lower floor Pd coating, and in lower floor Pd coating, Pd coating in the middle of attachment, middle Pd coating is adhered to upper strata Rh coating; Described lower floor 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), 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
3; In described lower floor Pd coating, the load capacity of Pd is 60g/ft
3, in middle Pd coating, the load capacity of Pd is 180g/ft
3, in the Rh coating of upper strata, the load capacity of Rh is 10g/ft
3;
The preparation method of described three-way catalyst, adopts following processing step:
The coating procedure of the 1st step, described lower floor Pd coating: by 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 mixing, and after ball milling preparation obtain coating slurry; Be coated on honeycomb support by this coating slurry, the coated weight of lower floor Pd coating is 100g/L, and 450 DEG C ~ 600 DEG C 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
3with the Y of 5wt%
2o
3;
The coating procedure of the 2nd step, described middle Pd coating: by 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%), 400 zirconium oxyacetate solution are (containing the ZrO of 84g
2) and appropriate amount of deionized water mixing, and preparation obtains coating slurry after ball milling; This coating slurry is coated to the 1st step complete after honeycomb support on, the coated weight of middle Pd coating is 100g/L, and 450 DEG C ~ 600 DEG C roasting temperatures 1 ~ 5 hour, obtains middle Pd coating;
The coating procedure of the 3rd step, described upper strata Rh coating: by 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 mixing, and after ball milling preparation obtain coating slurry; This coating slurry is coated to the 2nd step complete after honeycomb support on, upper strata Rh coating be applied to 160g/L, and 450 DEG C ~ 600 DEG C 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
3with the Y of 5wt%
2o
3.
Comparative example 1: each parameter, composition are identical with embodiment 1 with preparation process, except not containing the middle Pd coating in embodiment 1, and the coated weight of lower floor Pd coating becomes 120g/L, and the load capacity of Pd becomes 36g/ft
3.
Comparative example 2: each parameter, composition are identical with embodiment 1 with preparation process, except not containing the lower floor Pd coating in embodiment 1, and the coated weight of middle level Pd coating becomes 120g/L, and the load capacity of Pd becomes 36g/ft
3.
The catalyst sample that embodiment 1 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, adopt Electronic probe x-ray microregion analysis instrument (EPMA) to analyze the distribution proportion situation of Rh in each coating of catalyst, result is as shown in table 1.
Table 1
| Lower floor Pd coating | Middle Pd coating | Upper strata Rh coating | |
| Embodiment 1 | 6% | 16% | 78% |
| Comparative example 1 | 41% | —— | 59% |
| Comparative example 2 | —— | 17% | 83% |
Car load emission test is undertaken by ECE+EUDC circulation, and the engine displacement 1.8L of testing vehicle, 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 example 1 | 0.0501 | 0.691 | 0.0580 |
| Comparative example 2 | 0.0477 | 1.013 | 0.0739 |
As shown in table, table 2, the result of catalyst performance test and evaluation shows, compared with comparative example 1,2, three-way catalyst disclosed in the embodiment of the present invention 1 inhibits Rh to the migration of Pd layer, also possesses high oxygen storage power simultaneously, catalyst is made to have higher pollutant disposal ability, especially more excellent oxynitrides conversion capability.
Claims (7)
1. for a three-way catalyst for vehicle maintenance service, comprise honeycomb support, it is characterized in that: on described honeycomb support, adhere to lower floor Pd coating, in lower floor Pd coating, Pd coating in the middle of attachment, middle Pd coating is adhered to upper strata Rh coating; Described lower floor 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), 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 described lower floor Pd coating, the cerium zirconium sosoloid of load P d and La
2o
3-Al
2o
3mass ratio be 1 ~ 3:1;
In described middle Pd coating, binding agent accounts for the 1wt% ~ 10wt% of middle Pd coating gross mass;
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.
2., as claimed in claim 1 for the three-way catalyst of vehicle maintenance service, it is characterized in that: 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.
3., as claimed in claim 1 for the three-way catalyst of vehicle maintenance service, it is characterized in that: in described lower floor Pd coating, the load capacity of Pd is 5 ~ 200g/ft
3, in middle Pd coating, the load capacity of Pd is 5 ~ 200g/ft
3, in the Rh coating of upper strata, the load capacity of Rh is 0.1 ~ 10g/ft
3.
4. as claimed in claim 3 for the three-way catalyst of vehicle maintenance service, it is characterized in that: in described lower floor Pd coating and middle Pd coating, the mass ratio of the Pd of load is 3:1 ~ 9.
5., as claimed in claim 1 for the three-way catalyst of vehicle maintenance service, it is characterized in that: the coated weight of described lower floor Pd 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.
6., as claimed in claim 1 for the three-way catalyst of vehicle maintenance service, it is characterized in that: described La
2o
3-Al
2o
3in La
2o
3content accounts for La
2o
3-Al
2o
32wt% ~ 10wt%.
7., as claimed in claim 1 for the three-way catalyst of vehicle maintenance service, it is characterized in that: described binding agent is ZrO
2.
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|---|---|---|---|
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|---|---|---|---|
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| 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 |
| US20190136730A1 (en) * | 2016-06-07 | 2019-05-09 | Cataler Corporation | Exhaust gas purification catalyst |
| CN107597112A (en) * | 2017-08-16 | 2018-01-19 | 柳州申通汽车科技有限公司 | A kind of automobile using three-way catalyst |
| 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 |
| 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 |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| AU2006200894A1 (en) * | 2000-07-21 | 2006-03-30 | Johnson Matthey Public Limited Company | Hydrocarbon trap/catalyst composition |
| WO2009020957A1 (en) * | 2007-08-09 | 2009-02-12 | Basf Catalysts Llc | Multilayered catalyst compositions |
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| JP3591667B2 (en) * | 1995-06-23 | 2004-11-24 | 日野自動車株式会社 | NOx catalyst for purifying exhaust gas and method for producing the same |
| JP4240011B2 (en) * | 2005-06-20 | 2009-03-18 | トヨタ自動車株式会社 | Exhaust gas purification catalyst |
| JP4838258B2 (en) * | 2005-10-05 | 2011-12-14 | 株式会社キャタラー | Exhaust gas purification catalyst |
| CN101249438B (en) * | 2008-03-21 | 2011-08-17 | 无锡威孚环保催化剂有限公司 | Metallic composite oxides material with three hiberarchy and manufacture method thereof |
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Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| AU2006200894A1 (en) * | 2000-07-21 | 2006-03-30 | Johnson Matthey Public Limited Company | Hydrocarbon trap/catalyst composition |
| WO2009020957A1 (en) * | 2007-08-09 | 2009-02-12 | Basf Catalysts Llc | Multilayered catalyst compositions |
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