CN103007955A - Cleaning catalyst for automobile exhaust and preparation method of cleaning catalyst carrier - Google Patents
Cleaning catalyst for automobile exhaust and preparation method of cleaning catalyst carrier Download PDFInfo
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- CN103007955A CN103007955A CN201210571582XA CN201210571582A CN103007955A CN 103007955 A CN103007955 A CN 103007955A CN 201210571582X A CN201210571582X A CN 201210571582XA CN 201210571582 A CN201210571582 A CN 201210571582A CN 103007955 A CN103007955 A CN 103007955A
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Abstract
The invention provides a cleaning catalyst for automobile exhaust and a preparation method of a cleaning catalyst carrier. The catalyst comprises a carrier, an aid coating coated on the carrier, and an active ingredient loaded on the carrier coating, wherein the active ingredient is a mixed metallic oxide of yttrium, lanthanum, cerium, zirconium, manganese, copper and nickel; the carrier contains alumina and rare-earth lanthanum cerium oxide; and the aid coating is one or several oxides containing lanthanum, cerium, yttrium and zirconium. The preparation method of the carrier comprises the following steps of: hydrolyzing anhydrous aluminum chloride to prepare high-purity alumina, and preparing a saturated solution of lanthanum and cerium nitrate; adding the saturated solution into alumina, stirring, drying, grinding, mixing with graphite and polyethylene glycol, performing mold pressing and roasting. The catalyst has the characteristics that platinum, rhodium and other precious metals are not used, the cost is low, the activity is high, the heat, ageing and oxidization resistance capabilities are high, and the preparation process is simple.
Description
Technical field
The present invention relates to a kind of tail gas cleaning catalyst for vehicles and preparation method thereof, relate in particular to a kind of cleaning catalyst for tail gases of automobiles that does not use the noble metals such as platinum rhodium and preparation method thereof.
Background technology
Along with the car owning amount of China sharply increases, the vehicle exhaust pollution on the environment is also more and more serious.Just the auto-pollution control technology is carried out research and development research as far back as the sixties in 20th century abroad, reached at present the practical stage.Existing studies show that by performance and the production technology of improving catalyst and carrier thereof, improved car combustion engine combustion technology and catalyst gas extraction system, but purifying harmful gas.Catalytic cleaner wherein being installed, pernicious gas is processed, is the effective method of tail gas clean-up, and catalyst then is the key of clean-up effect.And catalyst is attached on the catalyst carrier, and the performance of catalyst carrier directly has influence on catalytic effect.
At present, the major measure of control motor vehicle exhaust emission is the purification techniques of the efficient auto-exhaust catalyst of exploitation.Currently use maximum auto-exhaust catalysts to be noble metal triple effect catalyst (TWC), noble metal catalyst has higher activity, and in the exhausted large ratio of world's tail-gas catalyst market share, but itself also has a lot of shortcomings.Only have when the scope control of air-fuel ratio when (14.6 ± 0.3), just can make NO
X, CO and HC detergent power reach maximum, outside this scope, catalytic effect is all relatively poor.The elements such as Pb, S, P all easily the time noble metal catalyst poison Pb having the greatest impact to TWC wherein.The price of noble metal is expensive, and at present the Precious Metals Resources scarcity also so that the application of TWC and popularization be restricted.
CN100396363C has reported a kind of three-way catalyst take the alumina load cerium zirconium sosoloid as carrier, and active component is Pd.Cerium zirconium sosoloid accounts for the 10-50wt% of catalyst quality, and the load capacity of Pd accounts for the 0.5-1.5% of catalyst quality.Its preparation method is the mixed solution of preparation cerium zirconium soluble-salt and citric acid, is impregnated into altogether on the alumina powder, obtains alumina load cerium zirconium compound oxide carrier through steps such as oven dry, roastings.Make Pd/CeZr/Al through steps such as oven dry, roasting, reduction behind the dipping precious metal solution
2O
3Three-way catalyst.
CN101773830A has reported a kind of preparation method of the high-temperature stability catalyst for catalytic cleaning of car tail gas, it is characterized in that prepared high-temperature stability material is the composite oxide solid solution that noble metal, cerium oxide, zirconia and auxiliary agent consist of.Compare the three-effect catalysis material that traditional infusion process obtains, the prepared catalyst of this invention can guarantee metal oxide containing precious metals stable existence under hot conditions, has good catalytic effect, can reach the standard of exhaust emissions.
Summary of the invention
Not high in order to overcome present domestic automobile tai-gas clean-up catalyst activity, the old oxidability of heat resistanceheat resistant is not strong, owing to use the noble metals such as platinum rhodium, the catalyst cost of manufacture is high, the problems such as preparation method complexity, make catalyst play better catalytic effect, reach the environmental requirement of in the world motor vehicle exhaust emission, the invention provides a kind of vehicle tail gas purification Catalysts and its preparation method, this catalyst has noble metals such as not using the platinum rhodium, and is with low cost, active high, the characteristics such as the old oxidability of heat resistanceheat resistant is strong, and manufacture craft is simple.
The present invention is used for the cleaning catalyst of vehicle exhaust, and this catalyst comprises carrier, be coated in the auxiliary agent coating on this carrier and be supported on active component on the described carrier coating.Described active component is the mixed-metal oxides of lanthanum cerium yttrium zirconium copper-manganese nickel, and described carrier contains aluminium oxide and Rare Earth Lanthanum cerium oxide, and described auxiliary agent coating is one or more oxides that contain lanthanum cerium yttrium zirconium.
Described active component is the mixed-metal oxides of lanthanum cerium yttrium zirconium copper-manganese nickel, and the weight of described active component is 2 ~ 8% of catalyst weight.
The weight ratio of lanthanum-cerium in the catalyst activity component-yttrium-zirconium-manganese-copper-nickel is 8 ~ 12: 30 ~ 36: 4 ~ 6: 28 ~ 32: 3 ~ 6: 5 ~ 8.Wherein, the content of lanthanum is 1.2 ~ 5.2g/L catalyst, and the content of cerium is 3.2 ~ 8.6g/L catalyst.
Described carrier wherein contains aluminium oxide and Rare Earth Lanthanum cerium oxide for the self-control carrier.The preparation method of described carrier comprises that the hydrolysis anhydrous Aluminum chloride prepares high purity aluminium oxide, and the nitrate saturated solution of configuration lanthanum cerium then adds in the aluminium oxide, stirs, and drying is ground, with roasting after graphite and the polyethylene glycol mixing mold pressing.
The weight ratio of aluminium oxide and Rare Earth Lanthanum cerium oxide is 1: 0.12 ~ 0.25, and lanthana is 1: 3 ~ 2: 1 to the weight ratio of cerium oxide in the Rare Earth Lanthanum cerium oxide.
The weight of auxiliary agent coating accounts for 10 ~ 30% of total catalyst weight.
The weight ratio of lanthanum-cerium in the auxiliary agent coating-yttrium-zirconium is 1 ~ 3: 3 ~ 5: 1 ~ 2: 2 ~ 6.
The preparation method of above-mentioned catalyst comprises:
(1) use oxyhydrogen flame hydrolysis 800g-1000g anhydrous Aluminum chloride to prepare pure alumina, to grind after the pure alumina drying that make, be immersed in the soluble barium salt solution of 0.5-1mol/L, filtration drying behind the dipping, heat treatment 3.5h in the time of 1000 ℃, the aluminium oxide after obtaining processing; (2) lanthanum nitrate hexahydrate: cerous nitrate solution: praseodymium chloride solution: the yttrium nitrate solution ratio is 1-3mol/L:1-2mol/L:0.5-1 mol/L:0.5-1 mol/L, be mixed with mixed solution of rare earth, add complexing agent, the weight ratio of used complexing agent and mixed solution of rare earth is 1:25, obtains precursor solution; Aluminium oxide after processing in the step (1) added in the described precursor solution stir, obtain the rare earth alumina mixed solution; (3) adding fine silica and aluminium oxide dispersant, adhesive obtain slurries in the rare earth alumina mixed solution, wherein the addition of fine silica in the rare earth alumina mixed solution is 2% ~ 5%(weight), the weight ratio 1-3 of aluminium oxide dispersant and adhesive; Slurries are 110-130 ℃ of drying, dried material is ground, heavy with 5-8%() active carbon and 1%(heavy) binding agent mix, again mixture is molded into the oval carrier that specification is T146.8 * 77 * 86.4, active carbon, dispersant, adhesive and binding agent are burnt in 600-800 ℃ of scope, obtain containing again the catalyst carrier of lanthanum cerium oxide in 22 hours 1200 ℃ of roastings.
It is characterized in that wherein the soluble barium salt solution described in the step (1) is barium nitrate, barium chloride or barium hydroxide.
It is characterized in that wherein the complexing agent described in the step (2) is citric acid, tartaric acid, ethylenediamine tetra-acetic acid or salicylic acid.
It is characterized in that wherein the aluminium oxide dispersant described in the step (3) is ammonium polymethacrylate, polyethylene glycol, calgon or trisodium citrate; Described adhesive is stearic acid, polyethylene glycol, polyacrylate or amino resins.
The characteristics such as the invention has the beneficial effects as follows: this catalyst has noble metals such as not using the platinum rhodium, and is with low cost, active high, and the old oxidability of heat resistanceheat resistant is strong, and manufacture craft is simple
Description of drawings
Fig. 1 is the transmission electron microscope photo of the catalyst of the carrier preparation of employing embodiment 1 preparation;
Fig. 2 is the transmission electron microscope photo of the catalyst of the carrier preparation of employing embodiment 2 preparations;
The specific embodiment
Embodiment 1
(1) uses oxyhydrogen flame hydrolysis 800g anhydrous Aluminum chloride to prepare pure alumina, will grind after the pure alumina drying that make, be immersed in the barium nitrate solution of 0.5mol/L filtration drying behind the dipping, heat treatment 3.5h in the time of 1000 ℃, the aluminium oxide after obtaining processing; (2) lanthanum nitrate hexahydrate: cerous nitrate solution: praseodymium chloride solution: the yttrium nitrate solution ratio is 1mol/L:1mol/L:0.5 mol/L:0.5 mol/L, be mixed with mixed solution of rare earth, add citric acid, the weight ratio of used citric acid and mixed solution of rare earth is 1:25, obtains precursor solution; Aluminium oxide after processing in the step (1) added in the described precursor solution stir, obtain the rare earth alumina mixed solution; (3) adding fine silica and aluminium oxide dispersant ammonium polymethacrylate, adhesive stearic acid obtain slurries in the rare earth alumina mixed solution, wherein the addition of fine silica in the rare earth alumina mixed solution is 2%(weight), the weight ratio 1 of aluminium oxide dispersant and adhesive; Slurries are 110 ℃ of dryings, dried material is ground, heavy with 5%() active carbon and 1%(heavy) binding agent mix, again mixture is molded into the oval carrier that specification is T146.8 * 77 * 86.4, active carbon, dispersant, adhesive and binding agent are burnt in 600 ℃ of scopes, obtain containing again the catalyst carrier of lanthanum cerium oxide in 22 hours 1200 ℃ of roastings.
Embodiment 2
(1) uses oxyhydrogen flame hydrolysis 1000g anhydrous Aluminum chloride to prepare pure alumina, will grind after the pure alumina drying that make, be immersed in the barium chloride solution of 1mol/L filtration drying behind the dipping, heat treatment 3.5h in the time of 1000 ℃, the aluminium oxide after obtaining processing; (2) lanthanum nitrate hexahydrate: cerous nitrate solution: praseodymium chloride solution: the yttrium nitrate solution ratio is 3mol/L:2mol/L:1 mol/L:1mol/L, be mixed with mixed solution of rare earth, add complexing agent tartaric acid, the weight ratio of used complexing agent and mixed solution of rare earth is 1:25, obtains precursor solution; Aluminium oxide after processing in the step (1) added in the described precursor solution stir, obtain the rare earth alumina mixed solution; (3) adding fine silica and aluminium oxide dispersant polyethylene glycol, adhesive polyacrylate obtain slurries in the rare earth alumina mixed solution, wherein the addition of fine silica in the rare earth alumina mixed solution is 5%(weight), the weight ratio 3 of aluminium oxide dispersant and adhesive; Slurries are 130 ℃ of dryings, dried material is ground, heavy with 8%() active carbon and 1%(heavy) binding agent mix, again mixture is molded into the oval carrier that specification is T146.8 * 77 * 86.4, active carbon, dispersant, adhesive and binding agent are burnt in 800 ℃ of scopes, obtain containing again the catalyst carrier of lanthanum cerium oxide in 22 hours 1200 ℃ of roastings.
Claims (5)
1. cleaning catalyst that is used for vehicle exhaust, this catalyst comprise carrier, be coated in the auxiliary agent coating on this carrier and be supported on active component on the described auxiliary agent coating, it is characterized in that:
Described active component is the mixed-metal oxides of lanthanum cerium yttrium zirconium copper-manganese nickel, the weight of stating active component is 2 ~ 8% of catalyst weight, the weight ratio of lanthanum-cerium in the catalyst activity component-yttrium-zirconium-manganese-copper-nickel is 8 ~ 12: 30 ~ 36: 4 ~ 6: 28 ~ 32: 3 ~ 6: 5 ~ 8, wherein, the content of lanthanum is 1.2 ~ 5.2g/L catalyst, the content of cerium is 3.2 ~ 8.6g/L catalyst;
Described carrier contains aluminium oxide and Rare Earth Lanthanum cerium oxide;
Described auxiliary agent coating is one or more oxides that contain lanthanum cerium yttrium zirconium, and the weight of auxiliary agent coating accounts for 10 ~ 30% of total catalyst weight, and the weight ratio of lanthanum-cerium-yttrium-zirconium is 1 ~ 3: 3 ~ 5 in the described auxiliary agent coating: 1 ~ 2: 2 ~ 6.
2. prepare the method for catalyst carrier claimed in claim 1, may further comprise the steps:
(1) use oxyhydrogen flame hydrolysis 800g-1000g anhydrous Aluminum chloride to prepare pure alumina, to grind after the pure alumina drying that make, be immersed in the soluble barium salt solution of 0.5-1mol/L, filtration drying behind the dipping, heat treatment 3.5h in the time of 1000 ℃, the aluminium oxide after obtaining processing;
(2) lanthanum nitrate hexahydrate: cerous nitrate solution: praseodymium chloride solution: the yttrium nitrate solution ratio is 1-3mol/L:1-2mol/L:0.5-1 mol/L:0.5-1 mol/L, be mixed with mixed solution of rare earth, add complexing agent (citric acid, tartaric acid, ethylenediamine tetra-acetic acid, salicylic acid), the weight ratio of used complexing agent and mixed solution of rare earth is 1:25, obtains precursor solution; Aluminium oxide after processing in the step (1) added in the described precursor solution stir, obtain the rare earth alumina mixed solution;
(3) adding fine silica and aluminium oxide dispersant, adhesive obtain slurries in the rare earth alumina mixed solution, wherein the addition of fine silica in the rare earth alumina mixed solution is 2% ~ 5%(weight), the weight ratio 1-3 of aluminium oxide dispersant and adhesive; Slurries are 110-130 ℃ of drying, dried material is ground, heavy with 5-8%() active carbon and 1%(heavy) binding agent mix, again mixture is molded into the oval carrier that specification is T146.8 * 77 * 86.4, active carbon, dispersant, adhesive and binding agent are burnt in 600-800 ℃ of scope, obtain containing again the catalyst carrier of lanthanum cerium oxide in 22 hours 1200 ℃ of roastings.
3. method according to claim 2 is characterized in that wherein the soluble barium salt solution described in the step (1) is barium nitrate, barium chloride or barium hydroxide.
4. method according to claim 2 is characterized in that wherein the complexing agent described in the step (2) is citric acid, tartaric acid, ethylenediamine tetra-acetic acid or salicylic acid.
5. method according to claim 2 is characterized in that wherein the aluminium oxide dispersant described in the step (3) is ammonium polymethacrylate, polyethylene glycol, calgon or trisodium citrate; Described adhesive is stearic acid, polyethylene glycol, polyacrylate or amino resins.
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103263925A (en) * | 2013-05-08 | 2013-08-28 | 上海纳米技术及应用国家工程研究中心有限公司 | Cerium-zirconium base nitric oxide common temperature catalyst preparation method |
| CN103638919A (en) * | 2013-12-20 | 2014-03-19 | 湖南稀土金属材料研究院 | Scandium-stabilized ceria-zirconia composite powder for automobile exhaust catalyst and preparation method thereof and automobile exhaust catalyst |
| CN103831101A (en) * | 2014-03-05 | 2014-06-04 | 浙江达峰汽车技术有限公司 | Catalyst coating capable of reducing POC (particle oxidation catalyst) regeneration temperature |
| CN108906072A (en) * | 2018-07-17 | 2018-11-30 | 无锡威孚环保催化剂有限公司 | A kind of diesel vehicle soot particle urges combustion catalyst and preparation method thereof |
| CN109046348A (en) * | 2018-08-24 | 2018-12-21 | 无锡威孚环保催化剂有限公司 | A kind of gasoline vehicle tail gas multicomponent catalyst and preparation method thereof |
| CN110064421A (en) * | 2018-01-23 | 2019-07-30 | 中国石油天然气股份有限公司 | A kind of reforming catalyst and preparation method thereof |
| CN110404536A (en) * | 2019-08-08 | 2019-11-05 | 无锡威孚环保催化剂有限公司 | The preparation method of the three-way catalyst of bilayer coating |
| CN114251158A (en) * | 2020-09-24 | 2022-03-29 | 广东加南环保生物科技有限公司 | Diesel exhaust particulate matter catalytic filter and method for manufacturing same |
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| CN1436592A (en) * | 2002-02-07 | 2003-08-20 | 中国石油化工股份有限公司 | Prepn process of catalyst for purfying automobile tail gas |
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Cited By (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103263925A (en) * | 2013-05-08 | 2013-08-28 | 上海纳米技术及应用国家工程研究中心有限公司 | Cerium-zirconium base nitric oxide common temperature catalyst preparation method |
| CN103638919A (en) * | 2013-12-20 | 2014-03-19 | 湖南稀土金属材料研究院 | Scandium-stabilized ceria-zirconia composite powder for automobile exhaust catalyst and preparation method thereof and automobile exhaust catalyst |
| CN103638919B (en) * | 2013-12-20 | 2016-08-17 | 湖南稀土金属材料研究院 | Auto-exhaust catalyst scandium stablizes cerium zirconium composite powder, its preparation method and auto-exhaust catalyst |
| CN103831101A (en) * | 2014-03-05 | 2014-06-04 | 浙江达峰汽车技术有限公司 | Catalyst coating capable of reducing POC (particle oxidation catalyst) regeneration temperature |
| CN103831101B (en) * | 2014-03-05 | 2016-08-24 | 浙江达峰汽车技术有限公司 | A kind of catalyst coat reducing POC regeneration temperature |
| CN110064421A (en) * | 2018-01-23 | 2019-07-30 | 中国石油天然气股份有限公司 | A kind of reforming catalyst and preparation method thereof |
| CN110064421B (en) * | 2018-01-23 | 2021-11-30 | 中国石油天然气股份有限公司 | Reforming catalyst and preparation method thereof |
| CN108906072A (en) * | 2018-07-17 | 2018-11-30 | 无锡威孚环保催化剂有限公司 | A kind of diesel vehicle soot particle urges combustion catalyst and preparation method thereof |
| CN109046348A (en) * | 2018-08-24 | 2018-12-21 | 无锡威孚环保催化剂有限公司 | A kind of gasoline vehicle tail gas multicomponent catalyst and preparation method thereof |
| CN110404536A (en) * | 2019-08-08 | 2019-11-05 | 无锡威孚环保催化剂有限公司 | The preparation method of the three-way catalyst of bilayer coating |
| CN114251158A (en) * | 2020-09-24 | 2022-03-29 | 广东加南环保生物科技有限公司 | Diesel exhaust particulate matter catalytic filter and method for manufacturing same |
| CN114251158B (en) * | 2020-09-24 | 2022-09-16 | 广东加南环保生物科技有限公司 | Diesel exhaust particulate matter catalytic filter and method for manufacturing same |
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