CN1973962A - RE perovskite type catalyst for oxidizing NO - Google Patents
RE perovskite type catalyst for oxidizing NO Download PDFInfo
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- CN1973962A CN1973962A CNA2005101240338A CN200510124033A CN1973962A CN 1973962 A CN1973962 A CN 1973962A CN A2005101240338 A CNA2005101240338 A CN A2005101240338A CN 200510124033 A CN200510124033 A CN 200510124033A CN 1973962 A CN1973962 A CN 1973962A
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- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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Abstract
The present invention relates to provides one kind of RE perovskite type catalyst for catalytic oxidation of NO into NO2, and features that the catalyst includes the perovskite type active component A1-xA'xB1-yB'yO3, where, A represents RE metal element La, A' includes Zr, Ce, Sr, Ca, Ba and Pr, B and B' represent transition metal element Fe, Co, Ni, Mn, Cu or Ti, x is 0-0.9, and y is 0-1.0. The catalyst of the present invention has simple preparation process, low cost, and NO oxidizing activity up to 80 % at 300 deg.c. It may be used to replace noble metal catalyst for oxidizing NO in lean combustion tail gas into NO2 to raise the NOx eliminating rate.
Description
Technical field
The present invention relates to a kind of RE perovskite type catalyst that the catalytic oxidation nitric oxide is a nitrogen dioxide that is used for.
Technical background
Because economic development and industrialized result, atmosphere pollution is serious day by day, especially the air quality severe exacerbation in city.In the various air pollutants, nitrogen oxide (NOx) is the very big pollutant of discharge capacity, is the key factor that forms acid rain and photochemical fog, and is harmful to entire environment and health.Nitrogen oxide is mainly derived from the burning of fuel.Along with the day by day reinforcement of countries in the world to Air Pollutant Emission control dynamics, several vent gas treatment technology at nitrogen oxide are developed, and comprise nitrogen oxide storage and reduction technology (NSR:the technique of NOx storage andreduction), nitrogen oxide and particle are removed technology (CRT:the continuously regenerated traptechnology for the simultaneous NOx and soot removal) simultaneously, the SCR technology of nitrogen oxide (SCR:the selective catalytic reduction of NOx) and at wet type nox adsorption technology of stationary source etc.NO
2As NO by O
2The product of oxidation is often effectively removed than the easier quilt of NO in above-mentioned technology, for example, in the wet absorption technology, the NO stable in properties, not soluble in water, be oxidized to NO
2, then dissolved efficiency improves greatly; In NSR technology, NO also must at first be oxidized to NO
2, could obtain storing in the form of catalyst surface with nitrate; In CRT technology, NO
2Compare O
2Oxidisability stronger, at first NO is oxidized to NO
2, the easier oxidized generation carbon dioxide of carbon soot particles, and NOx is reduced to N
2, reach simultaneously and remove; In the SCR process, NO is oxidized to NO
2Also be a requisite step in the reaction mechanism, NO
2Replacement NO is a reactant, can improve the utilization ratio of reducing agent greatly.
Yet in typical exhaust gas from diesel vehicle, NO
2The proportion that accounts for total NOx is very little, is about 5～10%.Obtain more NO
2, the catalyst of a kind of energy efficient oxidation NO is necessary.The oxidation of nitric oxide catalyst that generally uses at present is many to be active component with precious metals pt, loads on Al
2O
3On carrier, the load capacity of noble metal is generally 2～3%, the cost costliness, other then can not bear high temperature such as the catalyst that Fe loads on the molecular sieve, above drawbacks limit the more application of oxidation of nitric oxide catalyst under physical condition.
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 is provided, replace acquisition by the part of certain perovskite type rare earth complex oxide being carried out A position and B position.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 be in wider temperature range efficiently the catalytic oxidation nitric oxide be nitrogen dioxide.
Described catalyst comprises the Ca-Ti ore type active component shown in the following general formula:
A
1-xA’
xB
1-yB’
yO
3
A represents rare-earth metals La in the formula, and A ' comprises Zr, Ce, Sr, Ca, Ba, Pr; B and B ' represent transition metal Fe, Co, Ni, Mn, Cu and Ti; 0≤x≤0.9; 0≤y≤1.0.
The perovskite type composite oxide catalyst of the present invention's design can synthesize by several different methods, for example coprecipitation, direct evaporation, mechanical synthetic method, hydrothermal synthesis method, sol-gal process.Coprecipitation can be selected Na
2CO
3, different precipitating reagents such as ammoniacal liquor, urea.When using a kind of citric acid complex method that belongs to sol-gal process, selected metallic element can be mixed with citric acid solution by the design chemical dosage ratio with soluble compounds aqueous solution form, through fully stirring, at 60～80 ℃ of rotary evaporations that reduce pressure down, the dope that obtains is 120 ℃ of oven dry down, the reacted product dry powder of spontaneous combustion taking place through grinding mixing, calcined 1～3 hour down at 600～750 ℃, promptly obtains perovskite type composite oxide catalyst.The perovskite type catalyst that the present invention relates to has the specific area of 10～30 meters squared per gram, and average grain diameter is below 100 nanometers.
Aforesaid catalyst, can appendix on porous molecular screen, alundum (Al, silica, zirconia, cerium oxide and active carbon.According to different needs, can also make 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.
Preparation process of the present invention is simple, and is easy to operate.Compare with existing oxidation of nitric oxide catalyst, the present invention has following advantage:
1) mainly adopt rare earth metal and transition metal, abundant raw material need not noble metal, low cost of manufacture.
2) fabulous heat endurance.
3) outstanding catalysis oxidation of nitric oxide activity, the activity about 300 ℃ can reach 80%, reaches the dynamic (dynamical) limit of oxidation of nitric oxide reaction heat.
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
With lanthanum nitrate [La (NO
3)
36H
2O] 43.3 gram (0.100 mole), cobalt nitrate [Co (NO
3)
26H
2O] 29.1 grams (0.100 mole) are dissolved in 200 ml deionized water, fully stir.With citric acid [C
6H
8O
7H
2O] 42.0 grams (0.200 mole) are dissolved in the 100 ml deionized water solution fully and stir, and slowly pour into then in the metal salt solution, stir half an hour, pour in the pyriform glass flask, at 60～80 ℃ of rotary evaporations that reduce pressure down,, obtain the thickness complex compound with the moisture evaporate to dryness.This presoma is moved to evaporating dish, dry down in 120 ℃ and spend the night, obtain the dilated strong hygroscopic dry powder that has, after grinding, calcined 2 hours down, obtain the black powder sample at 700 ℃.
Identify that from the powder x-ray diffraction analysis result this powder is by LaCoO
3The single crystal that constitutes of the composite oxides of perovskite structure.Its specific area is 10 meters squared per gram.
Embodiment 2
With lanthanum nitrate [La (NO
3)
36H
2O] 34.6 gram (0.080 mole), cerous nitrate [Ce (NO
3)
36H
2O] 8.7 gram (0.020 mole), cobalt nitrate [Co (NO
3)
26H
2O] 29.1 grams (0.100 mole) are dissolved in 200 ml deionized water, fully stir.Other are operated similarly to Example 1, obtain the black powder sample.
Identify that from the powder x-ray diffraction analysis result this powder is by La
0.9Ce
0.1CoO
3Composite oxides and a small amount of CeO of perovskite structure
2And CoO
xThe mixture that constitutes.Specific area is 13 meters squared per gram.
Embodiment 3
With lanthanum nitrate [La (NO
3)
36H
2O] 26.0 gram (0.060 mole), cerous nitrate [Ce (NO
3)
36H
2O] 17.4 gram (0.040 mole), cobalt nitrate [Co (NO
3)
26H
2O] 14.6 gram (0.050 mole), nickel nitrate [Ni (NO
3)
26H
2O] 14.5 grams (0.050 mole) are dissolved in 200 ml deionized water, fully stir.Other are operated similarly to Example 1, obtain the black powder sample.
Identify that from the powder x-ray diffraction analysis result this powder is by La
0.9Ce
0.1Co
0.5Ni
0.5O
3Composite oxides and a small amount of CeO of perovskite structure
2, NiO
xAnd CoO
xThe mixture that constitutes.Specific area is 12 meters squared per gram.
Embodiment 4
With lanthanum nitrate [La (NO
3)
36H
2O] 26.0 gram (0.060 mole), cerous nitrate [Ce (NO
3)
36H
2O] 17.4 gram (0.040 mole), cobalt nitrate [Co (NO
3)
26H
2O] 14.6 gram (0.050 mole), nickel nitrate [Ni (NO
3)
26H
2O] 14.5 grams (0.050 mole) are dissolved in 200 milliliters of deionizations, fully stir.The ammoniacal liquor of 1 mol concentration is dropwise added in the metal salt solution, until precipitating fully.The gained presoma spends the night under 100 ℃, calcines 2 hours, and obtains the black powder sample for 700 ℃.
Identify that from the powder x-ray diffraction analysis result this powder is by La
0.9Ce
0.1Co
0.5Ni
0.5O
3The composite oxides and the more amount CeO of perovskite structure
2, NiO
xAnd CoO
xThe mixture that constitutes.Specific area is 10 meters squared per gram.
Comparative example 1
Get 100 gram γ-alundum (Al powder and be soaked in institute and decide in the chloroplatinic acid aqueous solution of concentration, stirred 1 hour, after 90 ℃ of dried overnight, in air, be warming up to 500 ℃ from 100 ℃ to stage, kept 3 hours, reduce to room temperature.The platinum component load capacity of manufactured goods catalyst is 2.0% (metallic element weight scaled value).
Comparative example 2
Cobalt nitrate [Co (NO3) 26H2O] 58.2 grams (0.200 mole) are dissolved in 200 ml deionized water, fully stir.Citric acid [C6H8O7H2O] 42.0 grams (0.400 mole) are dissolved in fully stirring in the 100 ml deionized water solution, slowly pour in the metal salt solution then, obtain mixed solution.Other operations are with embodiment 1.The gained powder is Co
3O
4
Above embodiment and the obtained catalyst of comparative example are respectively got 2.0 grams, be positioned over and carry out the catalyst activity evaluation experimental in the tubular fixed-bed reactor respectively, experiment condition is as follows:
Volume is formed: oxygen: 8%, and nitric oxide: 800ppm, helium: balance gas, total flow: 1250ml/min; The W/F:0.096gs/ml of reaction.
The activity rating result as shown in Figure 1.By result among the figure as can be known:
1) all embodiment gained catalyst can both reach the catalytic activity similar with comparative example 1, and wherein embodiment 2 gained catalyst activities are the highest.RE perovskite type catalyst of the present invention can be used for substituting the noble metal catalyst of respective negative carrying capacity.
2) comparative example 2 gained CATALYST Co
3O
4Catalytic activity far below the activity of such catalysts of above-mentioned all embodiment.
3) embodiment 2 is owing to added an amount of cerium in the A position, and activity improves a lot than embodiment 1.
4) even if under having added more the situation of volume cerium in the A position, the activity of embodiment 2 still is higher than embodiment 3, illustrates that the activity of cobalt on the B position is better than nickel.
5) comparing embodiment 3 and 4 as can be known, method for preparing catalyst also has certain influence to activity, citric acid complex method is better than using the coprecipitation of ammoniacal liquor as precipitating reagent.
Description of drawings
The described activity of such catalysts evaluation result of Fig. 1 embodiment and comparative example.
Claims (6)
1. one kind is used for the nitric oxide production RE perovskite type catalyst of catalytic oxidation, and can substitute noble metal catalyst and be used for before the purifying nitrogen oxides of lean-burn tail gas process, be nitric oxide pre-oxidation nitrogen dioxide, improve the removal efficient of nitrogen oxide.
2. catalyst as claimed in claim 1 is characterized in that described catalyst comprises the active component shown in the following Ca-Ti ore type general formula:
A
1-xA’
xB
1-yB’
yO
3
A represents rare-earth metals La in the formula, and A ' comprises Zr, Ce, Sr, Ca, Ba, Pr; B and B ' represent transition metal Fe, Co, Ni, Mn, Cu and Ti; 0≤x≤0.9; 0≤y≤1.0.
3. the described catalyst of claim 1 as described above can be by coprecipitation, directly evaporation, mechanical synthetic method, hydrothermal synthesis method, sol-gal process synthesize.
4. the described catalyst granules of claim 1 is Powdered as described above, has the specific area of 10～30 meters squared per gram, and average grain diameter is below 100 nanometers.
5. the described catalyst of claim 1 as described above, can appendix on porous molecular screen, alundum (Al, silica, zirconia, cerium oxide and active carbon.
6. the described catalyst of claim 1 as described above according to different needs, can be coated on the wall surface of ceramic honeycomb, metal mesh structure, open-celled foams.
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|---|---|---|---|
| CNA2005101240338A CN1973962A (en) | 2005-11-28 | 2005-11-28 | RE perovskite type catalyst for oxidizing NO |
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|---|---|---|---|
| CNA2005101240338A CN1973962A (en) | 2005-11-28 | 2005-11-28 | RE perovskite type catalyst for oxidizing NO |
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Cited By (19)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| 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 |
| US8128736B2 (en) | 2009-08-11 | 2012-03-06 | Linde Aktiengesellschaft | Carbon dioxide production for enhanced oil recovery |
| CN102397750A (en) * | 2010-09-14 | 2012-04-04 | 通用汽车环球科技运作有限责任公司 | Catalyst materials for nox oxidation in exhaust aftertreatment system that uses passive ammonia scr |
| CN102513087A (en) * | 2011-12-02 | 2012-06-27 | 中国科学院山西煤炭化学研究所 | Catalyst for synthesizing phenyl carbamate from diphenyl urea, preparation method and application |
| CN102989448A (en) * | 2012-12-18 | 2013-03-27 | 天津大学 | Preparation method and application of lanthanum-manganese perovskite type NOx removing catalyst |
| US20130259779A1 (en) * | 2012-03-30 | 2013-10-03 | GM Global Technology Operations LLC | Carbon monoxide-selective oxidation catalysts |
| CN103933969A (en) * | 2014-04-15 | 2014-07-23 | 华东理工大学 | Monolithic nitric oxide low-temperature oxidation catalyst and preparation method thereof |
| CN104415749A (en) * | 2013-08-22 | 2015-03-18 | 上海郎特汽车净化器有限公司 | SCR catalyst used for processing diesel-engine tail gas NOx and preparation method thereof |
| CN104689825A (en) * | 2015-02-12 | 2015-06-10 | 柳州豪祥特科技有限公司 | Method for preparing perovskite type mesoporous-alumina catalyst |
| CN105289639A (en) * | 2015-10-16 | 2016-02-03 | 上海纳米技术及应用国家工程研究中心有限公司 | Cobalt-loaded lanthanum, manganese, calcium and titanium ore type nitric oxide oxidation catalyst and preparation method |
| CN107591462A (en) * | 2017-09-26 | 2018-01-16 | 苏州英达瑞机器人科技有限公司 | A kind of flexible edge-sealing mechanism for the double glass battery component automatic edgers of solar energy |
| CN107999058A (en) * | 2016-11-01 | 2018-05-08 | 中国石油化工股份有限公司 | A kind of two-phase method flue-gas denitration process and denitration device |
| CN108745364A (en) * | 2018-05-15 | 2018-11-06 | 昆明理工大学 | A kind of preparation method of perovskite catalyst for catalytic oxidation NO |
| CN108745368A (en) * | 2018-05-15 | 2018-11-06 | 昆明理工大学 | A kind of double-perovskite catalyst and the preparation method and application 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 |
| CN111408379A (en) * | 2020-03-10 | 2020-07-14 | 武汉理工大学 | Purification treatment method for tail gas of diesel engine |
| CN112439406A (en) * | 2019-08-30 | 2021-03-05 | 大连海事大学 | Catalyst for catalytic oxidation of NO, preparation method and application thereof |
| CN114870848A (en) * | 2022-03-24 | 2022-08-09 | 桂林理工大学 | Tubular perovskite type composite oxide catalyst capable of reducing soot oxidation temperature of diesel engine |
| CN114984968A (en) * | 2022-07-08 | 2022-09-02 | 中国科学院生态环境研究中心 | Bifunctional catalyst with nitrogen oxide adsorption and oxidation functions as well as preparation method and application thereof |
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2005
- 2005-11-28 CN CNA2005101240338A patent/CN1973962A/en active Pending
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| 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 |
| US8128736B2 (en) | 2009-08-11 | 2012-03-06 | Linde Aktiengesellschaft | Carbon dioxide production for enhanced oil recovery |
| CN102397750A (en) * | 2010-09-14 | 2012-04-04 | 通用汽车环球科技运作有限责任公司 | Catalyst materials for nox oxidation in exhaust aftertreatment system that uses passive ammonia scr |
| CN102513087A (en) * | 2011-12-02 | 2012-06-27 | 中国科学院山西煤炭化学研究所 | Catalyst for synthesizing phenyl carbamate from diphenyl urea, preparation method and application |
| CN102513087B (en) * | 2011-12-02 | 2013-08-14 | 中国科学院山西煤炭化学研究所 | Catalyst for synthesizing phenyl carbamate from diphenyl urea, preparation method and application |
| US20130259779A1 (en) * | 2012-03-30 | 2013-10-03 | GM Global Technology Operations LLC | Carbon monoxide-selective oxidation catalysts |
| CN102989448A (en) * | 2012-12-18 | 2013-03-27 | 天津大学 | Preparation method and application of lanthanum-manganese perovskite type NOx removing catalyst |
| CN104415749A (en) * | 2013-08-22 | 2015-03-18 | 上海郎特汽车净化器有限公司 | SCR catalyst used for processing diesel-engine tail gas NOx and preparation method thereof |
| CN103933969B (en) * | 2014-04-15 | 2016-05-18 | 华东理工大学 | A kind of monolithic devices nitric oxide low-temperature oxidation catalyst and preparation method thereof |
| CN103933969A (en) * | 2014-04-15 | 2014-07-23 | 华东理工大学 | Monolithic nitric oxide low-temperature oxidation catalyst and preparation method thereof |
| CN104689825A (en) * | 2015-02-12 | 2015-06-10 | 柳州豪祥特科技有限公司 | Method for preparing perovskite type mesoporous-alumina catalyst |
| CN105289639A (en) * | 2015-10-16 | 2016-02-03 | 上海纳米技术及应用国家工程研究中心有限公司 | Cobalt-loaded lanthanum, manganese, calcium and titanium ore type nitric oxide oxidation catalyst and preparation method |
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| CN108745364A (en) * | 2018-05-15 | 2018-11-06 | 昆明理工大学 | A kind of preparation method of perovskite catalyst for catalytic oxidation NO |
| CN108745368A (en) * | 2018-05-15 | 2018-11-06 | 昆明理工大学 | A kind of double-perovskite catalyst and the preparation method and application 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 |
| CN112439406A (en) * | 2019-08-30 | 2021-03-05 | 大连海事大学 | Catalyst for catalytic oxidation of NO, preparation method and application thereof |
| CN112439406B (en) * | 2019-08-30 | 2023-11-03 | 大连海事大学 | Catalyst for catalytic oxidation of NO, and preparation method and application thereof |
| CN111408379A (en) * | 2020-03-10 | 2020-07-14 | 武汉理工大学 | Purification treatment method for tail gas of diesel engine |
| CN114870848A (en) * | 2022-03-24 | 2022-08-09 | 桂林理工大学 | Tubular perovskite type composite oxide catalyst capable of reducing soot oxidation temperature of diesel engine |
| CN114870848B (en) * | 2022-03-24 | 2023-08-11 | 桂林理工大学 | Tubular perovskite type composite oxide catalyst capable of reducing soot oxidation temperature of diesel engine |
| CN114984968A (en) * | 2022-07-08 | 2022-09-02 | 中国科学院生态环境研究中心 | Bifunctional catalyst with nitrogen oxide adsorption and oxidation functions as well as preparation method and application thereof |
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