CN109603823A - The lean-burn NO of diesel engine vent gas purification systemxTrap catalyst and preparation method thereof - Google Patents
The lean-burn NO of diesel engine vent gas purification systemxTrap catalyst and preparation method thereof Download PDFInfo
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Abstract
The present invention relates to a kind of lean-burn NO of diesel engine vent gas purification systemxTrap catalyst, is coated with bottom catalyst coat on the surface of catalyst carrier, is coated with overlying catalyst coating on the surface of bottom catalyst coat;Corresponding every liter of catalyst carrier includes the composite oxides of 200 ~ 300g, the barium monoxide of 10 ~ 30g, the precious metals pt of 1.0 ~ 3.0g and the precious metals pd of 0.4 ~ 0.7g in bottom catalyst coat;Corresponding every liter of catalyst carrier, includes composite oxides, the precious metals pt of 0.6 ~ 1.0g and the noble metal Rh of 0.15 ~ 0.25g of 30 ~ 60g in overlying catalyst coating;Composite oxides include ceria, aluminium oxide and other oxides;And other oxides are at least one of magnesia, zirconium oxide or lanthana.The present invention can not only the oxidizing fire hydro carbons (HC) and carbon monoxide (CO) that not exclusively generate, moreover it is possible to trapping and nitrogen oxides reduction (NOx).
Description
Technical field
The invention discloses a kind of lean-burn NO of diesel engine vent gas purification systemxTrap catalyst, the invention also discloses
A kind of lean-burn NOxThe preparation method of trap catalyst, the invention belongs to diesel motor exhaust cleaning catalyst technical fields.
Background technique
Diesel engine has fuel economy higher and CO as a kind of lean-burn automotive2The low advantage of discharge amount, makes
Diesel vehicle is especially more more and more universal in Europe in most of developed countries.But compared with stoichiometric gasoline engine,
The soot and NO of emission of diesel enginexIt is more, therefore the censure by vast public opinion.Diesel car engine is transported under lean-burn condition
It goes, the air-fuel ratio in tail gas is much larger than 14.7, and the clean-up effect of three-effect catalysis technology is unable to satisfy requirement in this case.At present
Applied to NO in exhaust gas from diesel vehiclexThe selective catalytic reduction technique of the mainstream technology of catalytic purification (SCR), lean-burn NOx trap
Technology (LNT) etc..
On the other hand, i.e., state's VI discharge standard of implementation is greatly reduced to the emission limit of NOx again, this is for diesel oil
Engine emission reduction work constitutes great challenge.For light-duty small displacement diesel engine, since cold start-up and idling etc. are low
The lower NO discharged of temperaturexIt can not be handled by SCR catalyst, therefore LNT is considered to have a kind of NO of Research ProspectsxCatalysis is net
Change post-processing technology.Compared to other techniques, LNT technology biggest advantage is not need additionally to add reducing agent, utilizes absorption
Memory technology has well solved low temperature NOxAnd the emission problem of unburned HC.LNT is the process of a cycle circulation,
The lean-burn stage is usually 1-2min in systems in practice, and the fuel-rich stage is 3-5s.In longer lean-burn stage (λ > 1), NOxFirst
It is adsorbed on catalyst surface, is then stored in the form of nitrite or nitrate on a catalyst, when reaction atmosphere switches
To of short duration fuel-rich stage (λ < 1), the NO of catalyst desorptionxBy H2, the reducibility gas such as CO, HC be reduced to N2Equal gases, and make
Catalyst is regenerated, and the circulation of next round is then proceeded by.
If CN102614875A discloses a kind of LNT catalyst applied for combining LNT-SCR, LNT catalyst is with firefly
The proton conductive oxide of stone structure, i.e. based on Ca (Sr)-La-Ce (Zr, Pr) mixed oxide, and further with Pt-Pd
Or Pt-Pd-Rh noble metal component combines.But even if these catalyst under low-speed (volume space velocity 10,000h-1),
NOx is not completely converted.
If CN102688691A discloses a kind of LNT catalyst that manganese-base oxide promotes, using containing MnOxBase metal
Oxide mixture (such as MnOx-CeO2) instead of the platinum in LNT system, with NOxStorage material and NOxReducing material combination makes
With.But these catalyst equally exist NOxThe low problem of transformation efficiency.
Therefore, lean-burn NOxThe NOx purifying property of trap catalyst is there is still a need for improving, to realize high NOxTransformation efficiency.
Summary of the invention
An object of the present invention is to overcome the deficiencies in the prior art, provide one kind can oxidizing fire it is incomplete
The hydro carbons (HC) and carbon monoxide (CO) of generation can simultaneously trap and nitrogen oxides reduction (NOx) diesel engine vent gas purification system
Lean-burn NOxTrap catalyst.
It is a further object of the present invention to provide a kind of lean-burn NO of diesel engine vent gas purification systemxThe preparation of trap catalyst
Method.
According to technical solution provided by the invention, the lean-burn NO of the diesel engine vent gas purification systemxTrap catalyst,
The surface of catalyst carrier is coated with bottom catalyst coat, applies on the surface of bottom catalyst coat coated with overlying catalyst
Layer;Corresponding every liter of catalyst carrier, the oxygen of composite oxides, 10~30g in bottom catalyst coat comprising 200~300g
Change barium, the precious metals pt of 1.0~3.0g and the precious metals pd of 0.4~0.7g;Corresponding every liter of catalyst carrier, in overlying catalyst
It include composite oxides, the precious metals pt of 0.6~1.0g and the noble metal Rh of 0.15~0.25g of 30~60g in coating;
The composite oxides include ceria, aluminium oxide and other oxides;And other oxides are magnesia, oxygen
Change at least one of zirconium or lanthana.
As preferred: the catalyst carrier is that cordierite honeycomb ceramic or iron-chromium-aluminum metal honeycomb, hole density exist
100-600 mesh/square inch.
As preferred: in the composite oxides, the weight ratio of ceria, aluminium oxide and other oxides is (3-
6):(3-6):(0.1-2)。
A kind of lean-burn NO of diesel engine vent gas purification systemxThe preparation method of trap catalyst the following steps are included:
A, at least one of magnesium nitrate, zirconium nitrate or lanthanum nitrate are impregnated on aluminium oxide together with cerous nitrate, it is quiet
It sets 8~12 hours, is then dried at 120~140 DEG C 7~9 hours, finally roast 2~3 hours, obtain at 500~600 DEG C
Mixed oxide;
B, the mixture that step a is obtained is weighed as required, and the presoma of mixed oxide, barium monoxide is added to deionization
In water, stir evenly, formed slurries, institute weighed mixed oxide quality and deionized water quality ratio be (1~2):
3, the slurries are handled with ball-milling technology, granularity D90 is controlled at 10 μm, platinum nitrate solution and nitric acid is added in the slurries
Slurries are all coated in catalyst carrier by palladium solution after mixing evenly, 8~12 hours dry at 120~140 DEG C, most
It is roasted 2~3 hours at 500~600 DEG C afterwards, is covered with bottom catalyst coat so that applying on the surface of catalyst carrier;
C, the mixed oxide that step a is obtained is weighed as required, mixed oxide is add to deionized water, and stirring is equal
It is even, formed slurries, the quality of the deionized water and institute the quality of weighed mixed oxide ratio be (1~2): 3;Through ball milling
Make 10 μm of granularity D90 of slurries, platinum nitrate solution and rhodium nitrate solution is then added in the slurries, after mixing evenly
Slurries are all coated to by bottom catalyst coat made from step b, are dried 7~9 hours at 120~140 DEG C,
500~600 DEG C roast 2~3 hours to get lean-burn NOx trap catalyst is arrived.
As preferred: the presoma of the barium monoxide is barium acetate or barium hydroxide.
The present invention can not only the oxidizing fire hydro carbons (HC) and carbon monoxide (CO) that not exclusively generate, moreover it is possible to trapping and also
Former nitrogen oxides (NOx)。
Specific embodiment
The present invention is further explained in the light of specific embodiments.
Embodiment 1
A kind of lean-burn NO of diesel engine vent gas purification systemxTrap catalyst, catalyst carrier are carrier cordierite ceramic,
The volume of catalyst carrier is 0.73L, and the hole density of catalyst carrier is 400 mesh/square inch;On the surface of catalyst carrier
Coated with bottom catalyst coat, overlying catalyst coating is coated on the surface of bottom catalyst coat;Corresponding every liter of catalysis
Agent carrier aoxidizes in bottom catalyst coat comprising cerium-magnesium-aluminum complex oxide comprising 227.3 grams per liters, 20 grams per liters
Barium, 2.25 grams per liter Pt and 0.45 grams per liter Pd;Corresponding every liter of catalyst carrier, in overlying catalyst coating comprising 49.1 grams/
Cerium-magnesium-aluminum complex oxide, 0.72 grams per liter Pt and the 0.18 grams per liter Rh risen;And the weight of cerium oxide, magnesia and aluminium oxide
Than for 4:1:5.
The lean-burn NO of above-mentioned diesel engine vent gas purification systemxTrap catalyst the preparation method is as follows:
A, it is small that 8 are then allowed to stand by magnesium nitrate and cerous nitrate co-impregnation to aluminium oxide using the method for incipient impregnation
When, it dries 7 hours at 120 DEG C, obtains mixed oxide after last 500 DEG C of roastings 2 hours;
B, the mixed oxide that step a is obtained is weighed as required, and weighed mixed oxide, barium acetate are added to 380g
It in deionized water, stirring evenly, forms slurries, handle the slurries with ball-milling technology, granularity D90 is at 10 μm or so for control,
Then platinum nitrate solution and palladium nitrate solution are added in the slurries, slurries are all coated to catalyst load after mixing evenly
8 hours dry at 120 DEG C on body, 500 DEG C roast 2 hours, are covered with bottom catalyst so that applying on the surface of catalyst carrier
Coating;
C, the mixed oxide that step a is obtained is weighed as required and is added in 143.4g deionized water, is stirred evenly, shape
At slurries;Make 10 μm of granularity D90 or so of slurries through ball milling, platinum nitrate solution and nitric acid are then added in the slurries
Slurries are coated on bottom catalyst coat by rhodium solution after mixing evenly, 7 hours dry at 120 DEG C, and 500 DEG C of roastings 2 are small
When, so that overlying catalyst coating is formed on bottom catalyst coat to get lean-burn NO is arrivedxTrap catalyst.
Embodiment 2
A kind of lean-burn NO of diesel engine vent gas purification systemxTrap catalyst, catalyst carrier are carrier cordierite ceramic,
The volume of catalyst carrier is 0.73L, and the hole density of catalyst carrier is 100 mesh/square inch;On the surface of catalyst carrier
Coated with bottom catalyst coat, overlying catalyst coating is coated on the surface of bottom catalyst coat;Corresponding every liter of catalysis
Agent carrier aoxidizes in bottom catalyst coat comprising cerium-zirconium-lanthanum-aluminium composite oxide comprising 227 grams per liters, 20 grams per liters
Barium, 2.25 grams per liter Pt and 0.45 grams per liter Pd;Corresponding every liter of catalyst carrier includes 50 grams per liters in overlying catalyst coating
Cerium-zirconium-lanthanum-aluminium composite oxide, 0.72 grams per liter Pt and 0.18 grams per liter Rh;And cerium oxide, zirconium oxide, lanthana and oxidation
The weight ratio of aluminium is 3:0.05:0.05:3.
The lean-burn NO of above-mentioned diesel engine vent gas purification systemxTrap catalyst the preparation method is as follows:
A, then quiet by zirconium nitrate, lanthanum nitrate and cerous nitrate co-impregnation to aluminium oxide using the method for incipient impregnation
It sets and is dried 8 hours at 10 hours, 130 DEG C, obtain mixed oxide after last 550 DEG C of roastings 2.5 hours;
B, the mixed oxide that step a is obtained is weighed as required, and weighed mixed oxide, barium hydroxide are added to
It in 380g deionized water, stirs evenly, forms slurries, handle the slurries with ball-milling technology, control granularity D90 on 10 μm of left sides
Then platinum nitrate solution and palladium nitrate solution are added in the slurries, slurries are all coated to catalysis after mixing evenly for the right side
10 hours dry at 130 DEG C on agent carrier, 550 DEG C roast 2.5 hours, are covered with bottom so that applying on the surface of catalyst carrier
Layer catalyst coat;
C, the mixed oxide that step a is obtained is weighed as required and is added in 143g deionized water, is stirred evenly, and is formed
Slurries;Make 10 μm of granularity D90 or so of slurries through ball milling, platinum nitrate solution and rhodium nitrate are then added in the slurries
Slurries are coated on bottom catalyst coat by solution after mixing evenly, 8 hours dry at 130 DEG C, and 550 DEG C of roastings 2.5 are small
When, so that overlying catalyst coating is formed on bottom catalyst coat to get lean-burn NO is arrivedxTrap catalyst.
Embodiment 3
A kind of lean-burn NO of diesel engine vent gas purification systemxTrap catalyst, catalyst carrier are carrier cordierite ceramic,
The volume of catalyst carrier is 0.73L, and the hole density of catalyst carrier is 600 mesh/square inch;On the surface of catalyst carrier
Coated with bottom catalyst coat, overlying catalyst coating is coated on the surface of bottom catalyst coat;Corresponding every liter of catalysis
Agent carrier includes cerium-magnesium-zirconium-lanthanum-aluminium composite oxide, 20 grams per liter oxygen comprising 227 grams per liters in bottom catalyst coat
Change barium, 2.25 grams per liter Pt and 0.45 grams per liter Pd;Corresponding every liter of catalyst carrier, in overlying catalyst coating comprising 50 grams/
Cerium-magnesium-lanthanum-aluminium composite oxide, 0.72 grams per liter Pt and the 0.18 grams per liter Rh risen;And cerium oxide, magnesia, zirconium oxide, oxygen
The weight ratio for changing lanthanum and aluminium oxide is 6:0.06:0.06:0.08:6.
The lean-burn NO of above-mentioned diesel engine vent gas purification systemxTrap catalyst the preparation method is as follows:
A, using the method for incipient impregnation, by magnesium nitrate, zirconium nitrate, lanthanum nitrate and cerous nitrate co-impregnation to aluminium oxide
On, it is then allowed to stand at 12 hours, 140 DEG C and dries 9 hours, obtain mixed oxide after last 600 DEG C of roastings 3 hours;
B, the mixed oxide that step a is obtained is weighed as required, and weighed mixed oxide, barium acetate are added to 380g
It in deionized water, stirring evenly, forms slurries, handle the slurries with ball-milling technology, granularity D90 is at 10 μm or so for control,
Then platinum nitrate solution and palladium nitrate solution are added in the slurries, slurries are all coated to catalyst load after mixing evenly
12 hours dry at 140 DEG C on body, 600 DEG C roast 3 hours, are covered with bottom catalysis so that applying on the surface of catalyst carrier
Agent coating;
C, the mixed oxide that step a is obtained is weighed as required and is added in 143g deionized water, is stirred evenly, and is formed
Slurries;Make 10 μm of granularity D90 or so of slurries through ball milling, platinum nitrate solution and rhodium nitrate are then added in the slurries
Slurries are coated on bottom catalyst coat by solution after mixing evenly, 9 hours dry at 140 DEG C, and 600 DEG C of roastings 3 are small
When, so that overlying catalyst coating is formed on bottom catalyst coat to get lean-burn NO is arrivedxTrap catalyst.
NOxTransformation efficiency evaluation
Carry out 20 lean combustions/fuel-rich switching circulation NO respectively at 150,200,250,300,350,400 DEG CxTransformation efficiency
It evaluates, includes 250ppm NO, 10%O in lean-burn atmosphere2、1000ppm CO、300ppm C3H6, 5%H2O, 5%CO2, use N2
As Balance Air, duration 100s;Fuel-rich atmosphere includes 250ppm NO, 0.5%O2, 3%CO, 0.5%H2、900ppm
C3H6, 5%H2O, 5%CO2, N2As Balance Air, duration 10s.Volume space velocity is 80,000h-1.Use Fourier transform
Infrared spectroscopy (FTIR) analyzer detection outlet production concentration, thus calculates the average NO of 20 circulationsxTransformation efficiency.
Table 1 describes average NO of the 1-3 of the embodiment of the present invention under lean combustion/fuel-rich switching cycling conditionxTransformation efficiency.
At 150 and 200 DEG C, the NO of 3 embodimentsxConversion ratio is suitable, and respectively 17% and 78% or so;In 250-400 DEG C of temperature model
In enclosing, the NO of embodiment 1xConversion ratio highest, followed by embodiment 3, and in this temperature range, the NO of embodiment 1xConversion ratio
All 80% or more.Evaluation result shows to use cerium-magnesium-aluminum complex oxide as carrier to NOxConversion performance is better than use
Cerium-zirconium-aluminium composite oxide is as carrier;Compared to barium hydroxide, barium acetate is used to be conducive to mention as oxidation barium precursor
Rise the high temperature NO of LNT catalystxTransformation efficiency.
Table 1
NOxConversion ratio/% | Embodiment 1 | Embodiment 2 | Embodiment 3 |
150℃ | 16.0 | 17.6 | 16.9 |
200℃ | 77.6 | 78.3 | 79.3 |
250℃ | 91.1 | 87.8 | 91.6 |
300℃ | 92.1 | 86.9 | 90.8 |
350℃ | 89.9 | 74.4 | 85.5 |
400℃ | 81.2 | 69.9 | 72.0 |
Claims (5)
1. a kind of lean-burn NO of diesel engine vent gas purification systemxTrap catalyst, it is characterized in that: being applied on the surface of catalyst carrier
It is covered with bottom catalyst coat, is coated with overlying catalyst coating on the surface of bottom catalyst coat;Corresponding every liter of catalyst
Carrier, in bottom catalyst coat comprising the composite oxides of 200 ~ 300g, the barium monoxide of 10 ~ 30g, 1.0 ~ 3.0g your gold
Belong to the precious metals pd of Pt and 0.4 ~ 0.7g;Corresponding every liter of catalyst carrier, the answering comprising 30 ~ 60g in overlying catalyst coating
Close oxide, the precious metals pt of 0.6 ~ 1.0g and the noble metal Rh of 0.15 ~ 0.25g;
The composite oxides include ceria, aluminium oxide and other oxides;And other oxides are magnesia, zirconium oxide
Or at least one of lanthana.
2. the lean-burn NO of diesel engine vent gas purification system as described in claim 1xTrap catalyst, it is characterized in that: the catalysis
Agent carrier is cordierite honeycomb ceramic or iron-chromium-aluminum metal honeycomb, and hole density is in 100-600 mesh/square inch.
3. the lean-burn NO of diesel engine vent gas purification system as described in claim 1xTrap catalyst, it is characterized in that: described multiple
It closes in oxide, the weight ratio of ceria, aluminium oxide and other oxides is (3-6): (3-6): (0.1-2).
4. a kind of lean-burn NO of diesel engine vent gas purification systemxThe preparation method of trap catalyst the following steps are included:
A, at least one of magnesium nitrate, zirconium nitrate or lanthanum nitrate are impregnated on aluminium oxide together with cerous nitrate, standing 8 ~
It 12 hours, is then dried at 120 ~ 140 DEG C 7 ~ 9 hours, is finally roasted 2 ~ 3 hours at 500 ~ 600 DEG C, obtain mixed oxidization
Object;
B, the mixed oxide that step a is obtained is weighed as required, and the presoma of mixed oxide, barium monoxide is added to deionization
In water, stir evenly, formed slurries, institute weighed mixed oxide quality and deionized water quality ratio be (1 ~ 2): 3,
The slurries are handled with ball-milling technology, granularity D90 is controlled at 10 μm, platinum nitrate solution and palladium nitrate is added in the slurries
Slurries are all coated in catalyst carrier by solution after mixing evenly, 8 ~ 12 hours dry at 120 ~ 140 DEG C, are finally existed
It is roasted 2 ~ 3 hours at 500 ~ 600 DEG C, is covered with bottom catalyst coat so that applying on the surface of catalyst carrier;
C, the mixed oxide that step a is obtained is weighed as required, and mixed oxide is add to deionized water, is stirred evenly,
Formed slurries, institute weighed mixed oxide quality and deionized water quality ratio be (1 ~ 2): 3, make slurries through ball milling
Granularity D90 is 10 μm, platinum nitrate solution and rhodium nitrate solution is then added in the slurries, after mixing evenly by slurries
It is all coated to by bottom catalyst coat made from step b, is dried 7 ~ 9 hours at 120 ~ 140 DEG C, at 500 ~ 600 DEG C
2 ~ 3 hours are roasted to get lean-burn NOx trap catalyst is arrived.
5. the lean-burn NO of diesel engine vent gas purification system as claimed in claim 4xThe preparation method of trap catalyst, feature
Be: the presoma of the barium monoxide is barium acetate or barium hydroxide.
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CN111939906A (en) * | 2020-08-26 | 2020-11-17 | 无锡威孚环保催化剂有限公司 | Lean-burn NOx trapping catalyst |
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CN115445613A (en) * | 2022-08-11 | 2022-12-09 | 凯龙蓝烽新材料科技有限公司 | Coating for lean-burn CNG catalyst and preparation method thereof |
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