CN1714931A - The perovskite type rare earth complex oxide catalyst of catalytic decomposition NOx under the excess oxygen - Google Patents
The perovskite type rare earth complex oxide catalyst of catalytic decomposition NOx under the excess oxygen Download PDFInfo
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- CN1714931A CN1714931A CN 200410047974 CN200410047974A CN1714931A CN 1714931 A CN1714931 A CN 1714931A CN 200410047974 CN200410047974 CN 200410047974 CN 200410047974 A CN200410047974 A CN 200410047974A CN 1714931 A CN1714931 A CN 1714931A
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Abstract
The invention provides a kind of catalytic decomposition NOx that is used for, particularly catalytic decomposition NOx becomes the catalyst of oxygen and nitrogen under excess oxygen.It is characterized in that this catalyst is made of simple perovskite type rare earth complex oxide, perhaps carried noble metal component and/or other metal components constitute on perovskite type rare earth complex oxide.Aforementioned perovskite type rare earth complex oxide is A
1-xA
xB
1-yB
yO
3(A=La, A=Ce, Ca, Sr, Ba, K, Cs; B, B=Co, Mn, Fe, Ni, Cr, Zn, Cu, V, Ti, Y, Zr, Rh, Ru, Pt, Au, Pd, Ag; X=0-1; Y=0-1) mixture of one or more perovskite type rare earth complex oxides wherein.Aforementioned noble metal component can be at least a among the following noble metal group, and aforementioned other metal components can be at least a in following other metal groups.Noble metal group: platinum, ruthenium, gold, rhodium, palladium; Other metal groups: silver, copper, iron, calcium, titanium, zirconium, caesium, barium, tin, tungsten, zinc, molybdenum, cerium, lanthanum.Preparation of Catalyst of the present invention is simple, and can effectively be applied to catalytic decomposition NOx under the excess oxygen.Catalyst of the present invention can effectively be eliminated O
2Inhibitory action, can be at the O of broad
2Use in the range of concentrations.The selectivity of catalyst of the present invention nitrogen in effective operating temperature interval can be up to 80-90%.
Description
Technical field
The present invention is used for catalytic decomposition NOx, and particularly catalytic decomposition NOx becomes oxygen and nitrogen under excess oxygen.
Technical background
A large amount of NOx has caused serious atmosphere pollution in the exhaust of lean-burn automotive.At present, poisonous NOx is converted into harmless nitrogen mainly contains three kinds of methods, be i.e. non-selective catalytic reduction (NCR), SCR (SCR) and direct catalytic decomposition method.Wherein the NOx direct breakdown method is that NOx directly is decomposed into O
2And N
2, because method is simple, operating cost is low, is considered to the NOx removal methods of tool prospect.But, contain 10% O in the tail gas usually for poor burn engine
2Direct decomposition reaction has very strong inhibitory action for NOx.At present, the catalyst of catalytic decomposition NOx under the known excess oxygen, the resolution ratio of NOx generally is no more than 10%.
After early-stage Study person found that the perovskite type rare earth complex oxide catalyst has good catalytic activity to the elimination of NOx, perovskite type rare earth complex oxide just was considered to the good motor vehicle vent gas purification catalysis agent of a class.Because higher temperature (being higher than 500 ℃, is 700-800 ℃ to most of catalyst), down, the free oxygen desorption that causes of NO is very fast, makes that the direct decomposition of NOx becomes possibility under no reducing agent existence condition.Perovskite type rare earth complex oxide exactly goes out advantages of high catalytic activity to this reaction and display.
Summary of the invention
The present invention is directed to the problems referred to above, a kind of perovskite type rare earth complex oxide catalyst that is used for catalytic decomposition NOx under the excess oxygen is provided.Replace to obtain by the part of certain perovskite type rare earth complex oxide being carried out A position and B position, perhaps the perovskite type rare earth complex oxide catalyst of catalytic decomposition NOx under the excess oxygen that a certain amount of noble metal of perovskite type rare earth complex oxide load and/or the common metal of moulding obtained greater activity.The present invention is fully taking into account on the basis of previous studies, is carrying out the result of big quantity research.The catalyst that is provided can direct efficiently catalytic decomposition NOx be O in wider temperature range
2And N
2
Catalyst of the present invention is made of simple perovskite type rare earth complex oxide, also can load on the same perovskite type rare earth complex oxide simultaneously or with any sequencing and constitute, also can constitute by mixing in addition by the different perovskite type rare earth complex oxides of load respectively by the noble metal component of 0.1-5% (metallic element weight scaled value) and/or other metal components.Aforementioned noble metal component is at least a in noble metal group platinum, ruthenium, gold, rhodium, the palladium, and aforementioned other metal components can be at least a in metal group silver, copper, iron, calcium, titanium, zirconium, caesium, barium, tin, tungsten, zinc, molybdenum, cerium, the lanthanum.
The metal component of aforementioned catalyst can be the form of the oxide of this metal or this metal and any inorganic salts and do not change its effect.It is characterized in that noble metal component has the particle diameter of average 5-300 nanometer on perovskite type rare earth complex oxide, be preferably average 10-50 nanometer.Perovskite type rare earth complex oxide is A
1-xA
x' B
1-yB
y' O
3(A=La, A '=Ce, Ca, Sr, Ba, K, Cs; B, B
y'=Co, Mn, Fe, Ni, Cr, Zn, Cu, V, Ti, Y, Zr, Rh, Ru, Pt, Au, Pd, Ag; X=0-1; Y=0-1) mixture of one or more perovskite type rare earth complex oxides wherein.The form of aforesaid perovskite type rare earth complex oxide can be Powdered also can be the Any shape of machine-shaping in advance.
According to the present invention, perovskite type rare earth complex oxide prepares with methods such as complexing infusion process, coprecipitation, thermolysis process or mechanical mixture.Noble metal component and other metal components can be by usefulness soluble compound water solution separately with well-known infusion processes, and the precipitation method or sol-gel process are deposited on the aforesaid perovskite type rare earth complex oxide.During such as the use infusion process, selected perovskite type rare earth complex oxide can be soaked in noble metal and other metals soluble compounds aqueous solution separately, stirred 1-24 hour, 80-120 ℃ of drying, interim ground is warming up to 600 ℃ from 100 ℃ in air or nitrogen or hydrogen or vacuum.The granular size of noble metal component and other metal components can be controlled by adjusting factors such as temperature, time and atmosphere.According to the present invention, also can one or more metal components be carried on the perovskite type rare earth complex oxide by preceding method any order, press with all the other metal components of quadrat method load then.According to the present invention, noble metal component also can load on respectively on the different perovskite type rare earth complex oxides with other metal components and constitute catalyst by mixing.
Aforesaid catalyst according to different needs, can be made various structures, as be coated on the wall surface of ceramic honeycomb or metal mesh structure, or open-celled foams also can be as the structural carrier of catalyst.Also catalyst can be made spherical or tabular use.
Preparation process of the present invention is simple, and is easy to operate.Compare with prior art, the present invention has following advantage:
(1) Preparation of Catalyst of the present invention is simple, and can effectively be applied to catalytic decomposition NOx under the excess oxygen.
(2) catalyst of the present invention can effectively be eliminated O
2Inhibitory action, can be at the O of broad
2Use in the range of concentrations.
(3) selectivity of catalyst of the present invention nitrogen in effective operating temperature interval can be up to 80-90%.
In order to be illustrated more clearly in the present invention, enumerate following examples, but it there is not any restriction to scope of the present invention.
Embodiment 1
After by stoichiometric proportion the lanthanum nitrate of various components, cerous nitrate, cobalt nitrate, nickel nitrate solution being mixed, add an amount of citric acid complexing agent, normal temperature stirs down and made it abundant complexing in 1 hour.Complex compound behind the Rotary Evaporators evaporate to dryness promptly obtains embodiment 1 catalyst at 120 ℃ of dry 12h behind 700 ℃ of roasting 6h.
Embodiment 2
Get in 25 gram the foregoing descriptions 1 catalyst and be soaked in institute and decide in the silver nitrate aqueous solution of concentration, stirred 1 hour, after 90 ℃ of dried overnight, in air, be warming up to 600 ℃ from 100 ℃ to stage, kept 3 hours, reduce to room temperature, promptly obtain embodiment 2 catalyst.The silver components load capacity of manufactured goods catalyst is 1% (metallic element weight scaled value).
Embodiment 3
Get in 25 gram the foregoing descriptions 1 catalyst and be soaked in institute and decide in the copper nitrate aqueous solution of concentration, stirred 1 hour, after 90 ℃ of dried overnight, in air, be warming up to 600 ℃ from 100 ℃ to stage, kept 3 hours, reduce to room temperature, promptly obtain embodiment 3 catalyst.The copper component load capacity of manufactured goods catalyst is 1% (metallic element weight scaled value).
Embodiment 4
After by stoichiometric proportion the lanthanum nitrate of various components, cerous nitrate, manganese nitrate, nickel nitrate solution being mixed, add an amount of citric acid complexing agent, normal temperature stirs down and made it abundant complexing in 1 hour.Complex compound behind the Rotary Evaporators evaporate to dryness gets the perovskite type rare earth complex oxide catalyst at 120 ℃ of dry 12h behind 700 ℃ of roasting 6h.The interpolation of metal component Ag is undertaken by infusion process.Get 25 the gram above-mentioned perovskite type rare earth complex oxide catalyst be soaked in decide in the silver nitrate aqueous solution of concentration, stirred 1 hour, after 90 ℃ of dried overnight, interim ground is warming up to 600 ℃ from 100 ℃ in air, kept 3 hours, and reduced to room temperature, promptly obtain embodiment 4 catalyst.The silver components load capacity of manufactured goods catalyst is 1% (metallic element weight scaled value).
Embodiment 5
1.0 gram embodiment 1 catalyst are positioned in the tubular fixed-bed reactor react, experiment condition is as follows:
Volume is formed: oxygen: 8%, and nitric oxide: 1000ppm, helium: balance gas, reaction velocity (GHSV) is 30,000h
-1At 250 ℃, nitric oxide production conversion ratio is 40%, and the selectivity of nitrogen is 87%.At 350 ℃, nitric oxide production conversion ratio is 76%, and the selectivity of nitrogen is 82%.
Embodiment 6
1.0 gram embodiment 2 catalyst are positioned in the tubular fixed-bed reactor react, experiment condition is as follows:
Volume is formed: oxygen: 8%, and nitric oxide: 1000ppm, helium: balance gas, reaction velocity (GHSV) is 30,000h
-1At 250 ℃, nitric oxide production conversion ratio is 50%, and the selectivity of nitrogen is 90%.At 350 ℃, nitric oxide production conversion ratio is 85%, and the selectivity of nitrogen is 85%.
Embodiment 7
1.0 gram embodiment 3 catalyst are positioned in the tubular fixed-bed reactor react, experiment condition is as follows:
Volume is formed: oxygen: 8%, and nitric oxide: 1000ppm, helium: balance gas, reaction velocity (GHSV) is 30,000h
-1At 250 ℃, nitric oxide production conversion ratio is 30%, and the selectivity of nitrogen is 94%.At 350 ℃, nitric oxide production conversion ratio is 70%, and the selectivity of nitrogen is 90%.
Embodiment 8
1.0 gram embodiment 4 catalyst are positioned in the tubular fixed-bed reactor react, experiment condition is as follows:
Volume is formed: oxygen: 10%, and nitric oxide: 1000ppm, helium: balance gas, reaction velocity (GHSV) is 30,000h
-1At 350 ℃, nitric oxide production conversion ratio is 55%, and the selectivity of nitrogen is 90%.At 450 ℃, nitric oxide production conversion ratio is 87%, and the selectivity of nitrogen is 84%.
Claims (5)
1. the perovskite type rare earth complex oxide catalyst of a catalytic decomposition NOx under excess oxygen, it is characterized in that this catalyst is made of simple perovskite type rare earth complex oxide, perhaps carried noble metal component and/or other metal components constitute on perovskite type rare earth complex oxide.
2. the described catalyst of claim 1 as described above is characterized in that, aforementioned noble metal component can be at least a among the following noble metal group, and aforementioned other metal components can be at least a in following other metal groups.
Noble metal group: platinum, ruthenium, gold, rhodium, palladium
Other metal groups: silver, copper, iron, calcium, titanium, zirconium, caesium, barium, tin, tungsten, zinc, molybdenum, cerium, lanthanum
3. the described catalyst of claim 1 as described above, it is characterized in that, aforementioned noble metal component and other metal components can be simultaneously or are loaded on the same perovskite type rare earth complex oxide with any sequencing and to constitute catalyst, also can load on respectively on the different perovskite type rare earth complex oxides to constitute catalyst by mixing.
4. the described catalyst of claim 1 as described above is characterized in that the load capacity of the metal component on the aforementioned perovskite type rare earth complex oxide is 0.1-5% (a metallic element weight scaled value).
5. the described catalyst of claim 1 as described above is characterized in that aforementioned perovskite type rare earth complex oxide is A
1-xA
x' B
1-yB
y' O
3(A=La, A '=Ce, Ca, Sr, Ba, K, Cs; B, B '=Co, Mn, Fe, Ni, Cr, Zn, Cu, V, Ti, Y, Zr, Rh, Ru, Pt, Au, Pd, Ag; X=0-1; Y=0-1) mixture of one or more perovskite type rare earth complex oxides wherein.The form of aforesaid perovskite type rare earth complex oxide can be Powdered also can be the Any shape of machine-shaping in advance, perhaps be coated on the material that has been shaped.
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| CN 200410047974 CN1714931A (en) | 2004-06-14 | 2004-06-14 | The perovskite type rare earth complex oxide catalyst of catalytic decomposition NOx under the excess oxygen |
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| EP2191892A1 (en) * | 2007-08-22 | 2010-06-02 | Honda Motor Co., Ltd. | Exhaust gas purification catalyst and exhaust gas purification apparatus using the exhaust gas purification catalyst |
| CN101804353A (en) * | 2010-03-15 | 2010-08-18 | 南京大学 | Pure perovskite phase rare earth ferrite porous hollow sphere, preparation method and application thereof |
| CN101837291A (en) * | 2009-03-16 | 2010-09-22 | 通用汽车环球科技运作公司 | Sulfur tolerant perovskite supported catalyst |
| CN101848756A (en) * | 2007-11-07 | 2010-09-29 | 本田技研工业株式会社 | Exhaust gas cleaner |
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- 2004-06-14 CN CN 200410047974 patent/CN1714931A/en active Pending
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