CN103962127A - Method and catalyst for performing low-temperature catalytic combustion to eliminate chlorination aromatic hydrocarbon - Google Patents
Method and catalyst for performing low-temperature catalytic combustion to eliminate chlorination aromatic hydrocarbon Download PDFInfo
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- CN103962127A CN103962127A CN201410206299.6A CN201410206299A CN103962127A CN 103962127 A CN103962127 A CN 103962127A CN 201410206299 A CN201410206299 A CN 201410206299A CN 103962127 A CN103962127 A CN 103962127A
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Abstract
The invention relates to a catalyst for catalytically combusting chlorination aromatic hydrocarbon at low temperature. The catalyst is LaMnO3 with a perovskite structure doped with Sr, Ce, Mg, Al, Fe, Co, Ni and Cu. The catalyst is used for performing low-temperature catalytic combustion to eliminate chlorination aromatic hydrocarbon, is easy to prepare, low in cost, high in catalytic activity, good in heat stability and long in service life, does not have by-products or cause secondary pollution, and is particularly suitable for low-temperature catalytic combustion for eliminating chlorination aromatic hydrocarbon. In air, at relatively low reaction temperature, chlorination aromatic hydrocarbon in waste gas can be converted into carbon dioxide and hydrogen chloride, and completely combusted exhaust gas can be emptied after acid gases such as hydrogen chloride and chlorine are absorbed by a dilute alkali solution.
Description
Technical field
The invention belongs to catalytic combustion environmental technology field, specially refer to a kind of method and used catalyst of eliminating for chlorination aromatic hydrocarbon low-temperature catalytic burning.
Background technology
Chlorine-containing volatile organic compound (CVOCs) not only can cause serious harm to the mankind's health, also can cause lasting, cumulative impact, and can destroy atmospheric ozone layer to biosystem.Therefore, a lot of countries have formulated strict environmental legislation for the discharge of CVOCs now.Chlorine-containing volatile hydro carbons is divided into non-aromatic fat hydrocarbon chloride, as dichloroethanes, trichloro-ethylene, chloromethanes and methane polychloride etc., and aromatic hydrocarbon chloride, as chlorobenzene, dichloro-benzenes.The former results from chlorine industry oxygen chlorine legal system for industries such as vinyl chloride process, process hides, washing, pharmacy, and the latter results from bleaching, the heat treatment of chlorine-containing compound and the recovery of metal etc. of the wood pulp of chloro oxidant.Because the discharge process of these CVOCs is all the industrial process that concerns national economy, therefore the discharge of a large amount of CVOCs is inevitable, and therefore, the pollution of eliminating CVOCs from source does not possess possibility.And the pollution that adopts the method elimination CVOCs of post processing to bring becomes unique feasible approaches and methods.
At present a lot of about the method for the CVOCs comprehensive regulation, at present, for the removal of chlorinated organics, mainly contain the methods such as direct burning, absorption method, absorption process, photocatalysis, catalytic hydrogenation and dechlorination, catalyzed aqueous vapour reformation, catalytic combustion.It is low by (250 that catalytic combustion possesses operating temperature
oc-550
oc), wide, the product (CO of pollution abatement substrate concentration
2, HCl and H
2o) selective high.Therefore, catalytic combustion is being widely used aspect elimination volatile organic compound.
Chlorination aromatic hydrocarbon mainly results from Refuse Incineration Process as chlorobenzene, polystream He bioxin.Due to the hypertoxicity of these type of species, so the general presomas such as chlorobenzene, dichloro-benzenes and chlorophenol that adopt carry out screening of catalyst and investigation as Model Molecule under experiment condition.
Mainly concentrate on the catalyst of three types for CVOCs catalytic combustion: noble metal catalyst, solid acid catalyst, catalyst of transition metal oxide.Noble metal catalyst exists that price is relatively costly, chloro active high (easily producing many chloros accessory substance that toxicity is larger), easily generate oxychlorination compound and poisoning, in high-temperature region because of the loss of noble metal the problem such as poisoning, the application of noble metal catalyst is restricted.Mainly V for the transition-metal catalyst of chlorination aromatic hydrocarbon catalytic combustion at present
2o
5-TiO
2-catalyst based etc.But, V
2o
5-TiO
2-catalyst based middle TiO
2there is toxicity, easily cause secondary pollution, limited its application.Though the catalyst of other types is applied as solid acid catalyst has some, eventually do not promoted widely because activity is low or accessory substance is many.
In patent documentation, the main catalyst activity component transition metal oxide using is UO
2, MnO
2, Co
3o
4, La
2o
3, CeO
2deng and precious metals pt, Pd etc., carrier is SiO
2, Al
2o
3, TiO
2, ZrO
2.Representational patent has JP 2002219364, JP 2001286729, JP2001278630, JP 2001009284, JP 2001286734, JP 2001327869, JP 10085559A2, U. S. Patent 4031149, U. S. Patent 4059677, U. S. Patent 4065543, U. S. Patent 4561969, U. S. Patent 58116628, U. S. Patent 4169862, U. S. Patent 7052663 etc.
Summary of the invention
The object of the invention is to openly a kind of method for chlorination aromatic hydrocarbon low-temperature catalytic burning and catalyst, catalyst preparation is simple, with low cost, catalytic activity is high, no coupling product, does not cause secondary pollution, Heat stability is good, catalyst life is long, is specially adapted to the chloride aromatic hydrocarbon of low-temperature catalyzed elimination.
A first aspect of the present invention is a kind of catalyst of eliminating for chlorination aromatic hydrocarbon low-temperature catalytic burning, and it is the LaMnO of the perovskite structure of Sr, Ce, Mg, Al, Fe, Co, Ni, Cu doping
3.
Preferably, catalyst of the present invention is Sr, Ce, the Mg La position of adulterating, the LaMnO of the perovskite structure of Al, Fe, Co, Ni, Cu doped with Mn position
3, wherein doping is 20%.
Preferably, catalyst of the present invention adopts citric acid complex method, urea decomposition method, coprecipitation doped chemical to be doped to the LaMnO of perovskite structure
3in obtain.
Preferably, in the described coprecipitation of catalyst of the present invention, in the mixed aqueous solution taking the mixed solution of sodium carbonate and NaOH as coprecipitator is added drop-wise to described presoma nitrate, form precipitation, sediment is through 650-750
oc roasting obtains the LaMnO of the perovskite structure of doping
3.
A second aspect of the present invention is a kind of method that chlorination aromatic hydrocarbon low-temperature catalytic burning is eliminated, and it is using catalyst of the present invention as catalytic combustion catalyst.
Preferably, the inventive method comprises: under described catalyst exists, taking air as oxidant, make the chlorination aromatic hydrocarbon burning in discarded object, ignition temperature is 100-500
oc.
Preferably, in the inventive method, ignition temperature is 250-350
oc.
Preferably, the consumption of catalyst described in the inventive method is set to be enough to make chlorination aromatic hydrocarbon to change into carbon dioxide and hydrogen chloride.
Preferably, in the inventive method the consumption of catalyst to be set to every gram of catalyst treatment be 10-30L per hour containing the exhausted air quantity of the many chlorination aromatic hydrocarbons of 0.05-5vol%.
Adopt catalyst of the present invention, in air, under lower reaction temperature, the chlorination aromatic hydrocarbon in discarded can be changed into carbon dioxide and hydrogen chloride, the activity of catalyst does not reduce.
It is simple that catalyst provided by the invention has preparation, and with low cost, catalytic activity is high, and no coupling product does not cause secondary pollution, Heat stability is good, the features such as catalyst life length; Technology path is convenient and practical, can be widely used in the low-temperature catalyzed purification of the catalytic combustion of the chloride volatile organic contaminant in the industrial waste gases such as papermaking, pharmacy, process hides, washing, waste incineration.
Detailed description of the invention
Embodiment 1
Commercially available 2g NaOH and 5.3g sodium carbonate are dissolved in 100ml water and form mixed solution, as solution A; Commercially available 3.7g lanthanum nitrate hexahydrate is dissolved in 150ml water, adds 50% the manganese nitrate solution of 3.58g to form mixed solution, as solution B; At room temperature, under the condition of stirring, A solution is dropwise added drop-wise in B solution, forms precipitation, at room temperature in air, leave standstill 12h; Filtration obtains filter cake, and washing leaching cake is to PH=7 left and right, 110
oc oven drying 12h, takes out grind into powder, then moves to roasting in Muffle furnace.Its roasting process is: 50
oc starts heating, with 4
othe heating rate of C/min carries out temperature programming, is warming up to 650
oc, 650
oc keeps 5h, obtains the LaMnO of unadulterated perovskite structure
3catalyst, is denoted as LMO.
Embodiment 2
Commercially available 2g NaOH and 5.3g sodium carbonate are dissolved in 100ml water and form mixed solution, as solution A; The strontium nitrate of the lanthanum nitrate hexahydrate of commercially available 2.96g and 0.423g is dissolved in 150ml water, adds 50% the manganese nitrate solution of 3.58g to form mixed solution, as solution B; Other experimentation and embodiment 1 are consistent, and obtain the LaMnO of the perovskite structure of Sr doping
3catalyst, is denoted as LSMO.
Embodiment 3
Commercially available 2g NaOH and 5.3g sodium carbonate are dissolved in 100ml water and form mixed solution, as solution A; The six nitric hydrate ceriums of the lanthanum nitrate hexahydrate of commercially available 2.96g and 0.868g are dissolved in 150ml water, add 50% the manganese nitrate solution of 3.58g to form mixed solution, as solution B; Other experimentation and embodiment 1 are consistent, and obtain the LaMnO of the perovskite structure of Ce doping
3catalyst, is denoted as LCMO.
Embodiment 4
Commercially available 2g NaOH and 5.3g sodium carbonate are dissolved in 100ml water and form mixed solution, as solution A; The magnesium nitrate hexahydrate of the lanthanum nitrate hexahydrate of commercially available 2.96g and 0.513g is dissolved in 150ml water, adds 50% the manganese nitrate solution of 3.58g to form mixed solution, as solution B; Other experimentation and embodiment 1 are consistent, and obtain the LaMnO of the perovskite structure of Mg doping
3catalyst, is denoted as LMMO.
Embodiment 5
Commercially available 2g NaOH and 5.3g sodium carbonate are dissolved in 100ml water and form mixed solution, as solution A; The ANN aluminium nitrate nonahydrate of the lanthanum nitrate hexahydrate of commercially available 3.7g and 0.758g is dissolved in 150ml water, adds 50% the manganese nitrate solution of 2.86g to form mixed solution, as solution B; Other experimentation and embodiment 1 are consistent, and obtain the catalyst of the perovskite structure of Al doping, are denoted as LMAO.
Embodiment 6
Commercially available 2g NaOH and 5.3g sodium carbonate are dissolved in 100ml water and form mixed solution, as solution A; The Fe(NO3)39H2O of the lanthanum nitrate hexahydrate of commercially available 3.7g and 0.82g is dissolved in 150ml water, adds 50% the manganese nitrate solution of 2.86g to form mixed solution, as solution B; Other experimentation and embodiment 1 are consistent, and obtain the LaMnO of the perovskite structure of Fe doping
3catalyst, is denoted as LMFO.
Embodiment 7
Commercially available 2g NaOH and 5.3g sodium carbonate are dissolved in 100ml water and form mixed solution, as solution A; The cabaltous nitrate hexahydrate of the lanthanum nitrate hexahydrate of commercially available 3.7g and 0.582g is dissolved in 150ml water, adds 50% the manganese nitrate solution of 2.86g to form mixed solution, as solution B; Other experimentation and embodiment 1 are consistent, and obtain the LaMnO of the perovskite structure of Co doping
3catalyst, is denoted as LMCoO.
Embodiment 8
Commercially available 2g NaOH and 5.3g sodium carbonate are dissolved in 100ml water and form mixed solution, as solution A; The Nickelous nitrate hexahydrate of the lanthanum nitrate hexahydrate of commercially available 3.7g and 0.593g is dissolved in 150ml water, adds 50% the manganese nitrate solution of 2.86g to form mixed solution, as solution B; Other experimentation and embodiment 1 are consistent, and obtain the LaMnO of the perovskite structure of Ni doping
3catalyst, is denoted as LMNO.
Embodiment 9
Commercially available 2g NaOH and 5.3g sodium carbonate are dissolved in 100ml water and form mixed solution, as solution A; The Gerhardite of the lanthanum nitrate hexahydrate of commercially available 3.7g and 0.483g is dissolved in 150ml water, adds 50% the manganese nitrate solution of 2.86g to form mixed solution, as solution B; Other experimentation and embodiment 1 are consistent, and obtain the LaMnO of the perovskite structure of Cu doping
3catalyst, is denoted as LMCuO.
Embodiment 10
All catalyst activity evaluations for chlorobenzene catalytic combustion are carried out at fixed-bed micro-reactor (internal diameter 3mm quartz), and the consumption of catalyst is 200mg, and temperature adopts K type thermocouple automatically to control.Adopt 100 serial KDS120 type micro-injection pumps of Stoelting company of the U.S. that chlorobenzene injection is entered to vaporizer, be then mixed into reactor with air and burn.Total flow adopts mass flowmenter control, and the concentration of chlorobenzene is 0.1vol%, and the exhausted air quantity of every gram of catalyst processing per hour is 15L, is 100m/h through the linear velocity of the gas of reactor.Reaction pressure be the conversion ratio of 0.1MPa chlorobenzene and the relation of reaction temperature in table 1, T in table
10%, T
50%, T
90%be respectively conversion ratio required reaction temperature while reaching 10%, 50%, 90%.Key reaction product is carbon dioxide, hydrogen chloride and a small amount of chlorine.
Chlorobenzene catalytic combustion properties in table 1 different catalysts.
| Catalyst | T 10%( oC) | T 50%( oC) | T 90%(oC) |
| Embodiment 1 | 127 | 231 | 320 |
| Embodiment 2 | 109 | 196 | 289 |
| Embodiment 3 | 104 | 210 | 415 |
| Embodiment 4 | 114 | 214 | 393 |
| Embodiment 5 | 137 | 248 | 390 |
| Embodiment 6 | 170 | 260 | 495 |
| Embodiment 7 | 136 | 248 | 500 |
| Embodiment 8 | 148 | 267 | 500 |
| Embodiment 9 | 148 | 250 | 500 |
Embodiment 11
The concentration that changes chlorobenzene, the amount of every gram of catalyst processing waste gas per hour is 15L, reaction pressure, at 0.3MPa-0.5MPa, has been investigated the impact of the catalyst LSMO catalytic combustion properties of variable concentrations chlorobenzene on embodiment 3, the results are shown in Table 2.
The impact of table 2 variable concentrations chlorobenzene on LSMO catalyst combustion activity.
| Chlorobenzene concentration (vol%) | T 10%( oC) | T 50%( oC) | T 90%( oC) |
| 0.05 | 95 | 200 | 265 |
| 0.1 | 109 | 196 | 289 |
| 0.15 | 134 | 220 | 315 |
Result shows, embodiment 2 catalyst LSMO all have good catalytic combustion properties for higher or low concentration chlorobenzene.As can be seen here, the catalyst in the present invention can be widely used for the catalytic combustion elimination of the chlorination aromatic hydrocarbon of variable concentrations.
Embodiment 12
Adopt the evaluating catalyst system identical with embodiment 10, in the chlorobenzene reaction gas of 0.05vol%, introduce respectively the toluene of the normal heptane of 0.05vol% or the n-hexane of 0.05vol% or 0.05vol%, investigate the variation of embodiment 2 catalyst LSMO chlorobenzene catalytic combustion activity.
The impact of table 3 different hydrocarbons on LSMO catalyst combustion activity.
| The hydro carbons adding | T 10%( oC) | T 50%( oC) | T 90%( oC) |
| Normal heptane | 101 | 205 | 263 |
| N-hexane | 93 | 202 | 256 |
| Toluene | 106 | 216 | 268 |
It is very little that result shows that the introducing of normal heptane, n-hexane and toluene affects the degree of embodiment 2 catalyst LSMO catalytic activitys, shows that embodiment 2 catalyst LSMO can, in the various waste gas that contains hydrocarbon compound, eliminate chlorination aromatic hydrocarbon compounds effectively.
Embodiment 13
Adopt the evaluating catalyst system identical with embodiment 10, taking benzene as pollutant, pollutant levels are 0.1vol%, and the exhausted air quantity of every gram of catalyst processing per hour is 15L, are 100m/h through the linear velocity of the gas of reactor, and reaction pressure is 0.1MPa.The conversion ratio of benzene and the relation of reaction temperature be in table 4, T in table
10%, T
50%, T
90%be respectively conversion ratio required reaction temperature while reaching 10%, 50%, 90%.Key reaction product is carbon dioxide and water.
Benzene catalytic combustion activity in table 4 different catalysts.
| Catalyst | T 10%( oC) | T 50%( oC) | T 90%( oC) |
| Embodiment 1 | 111 | 226 | 290 |
| Embodiment 2 | 103 | 188 | 250 |
| Embodiment 3 | 123 | 196 | 260 |
| Embodiment 4 | 116 | 205 | 267 |
| Embodiment 5 | 114 | 250 | 300 |
| Embodiment 6 | 130 | 260 | 310 |
| Embodiment 7 | 123 | 251 | 317 |
| Embodiment 8 | 129 | 263 | 323 |
| Embodiment 9 | 131 | 257 | 316 |
Result shows to adopt the LaMnO of doping prepared by coprecipitation
3perovskite catalyst shows good catalytic oxidation activity for the catalytic combustion of benzene, and the especially LSMO catalyst in embodiment 2, has all shown very high catalytic oxidation activity for the catalytic combustion of benzene and chlorobenzene.This catalyst series can be applicable to various aromatic hydrocarbon and chlorination aromatic hydrocarbon waste gases processing.
Claims (10)
1. for a catalyst for chlorination aromatic hydrocarbon low-temperature catalytic burning, it is the LaMnO of the perovskite structure of Sr, Ce, Mg, Al, Fe, Co, Ni, Cu doping
3.
2. catalyst as claimed in claim 1, it is Sr, Ce, the Mg La position of adulterating, the LaMnO of the perovskite structure of Al, Fe, Co, Ni, Cu doped with Mn position
3, wherein doping is 20%.
3. catalyst as claimed in claim 1, adopts citric acid complex method, urea decomposition method, coprecipitation that doped chemical is doped to LaMnO
3in perovskite structure, obtain.
4. catalyst as claimed in claim 1, as presoma, adopts coprecipitation preparation with the slaine that is selected from nitrate, oxalates, acetate and carbonate.
5. catalyst as claimed in claim 4, in described coprecipitation: form precipitation in the mixed aqueous solution taking the mixed solution of sodium carbonate and NaOH as coprecipitator is added drop-wise to described presoma nitrate, sediment obtains the LaMnO of the perovskite structure of doping through 650-750oC roasting
3.
6. the method that chlorination aromatic hydrocarbon low-temperature catalytic burning is eliminated, is characterized in that, using the catalyst described in claim 1-5 any one as catalytic combustion catalyst.
7. method as claimed in claim 6, comprising: under described catalyst exists, taking air as oxidant, make the chlorination aromatic hydrocarbon burning in discarded object, ignition temperature is 100-500oC.
8. method as claimed in claim 7, wherein ignition temperature is 250-350oC.
9. method as claimed in claim 8, the consumption of described catalyst is set to be enough to make chlorination aromatic hydrocarbon to change into carbon dioxide and hydrogen chloride.
10. method as claimed in claim 9, it is 10-30L per hour containing the exhausted air quantity of 0.05-5vol% chlorination aromatic hydrocarbon that the consumption of described catalyst is set to every gram of catalyst treatment.
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| CN106994348A (en) * | 2017-03-22 | 2017-08-01 | 华东理工大学 | It is a kind of for catalyst of chlorination aromatic hydrocarbon low-temperature catalytic burning and its preparation method and application |
| CN107456964A (en) * | 2017-08-23 | 2017-12-12 | 清华大学 | For the extra specific surface area perovskite type composite oxide catalyst of hydrocarbon low-temperature oxidation and its preparation |
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| CN106994348A (en) * | 2017-03-22 | 2017-08-01 | 华东理工大学 | It is a kind of for catalyst of chlorination aromatic hydrocarbon low-temperature catalytic burning and its preparation method and application |
| CN107456964A (en) * | 2017-08-23 | 2017-12-12 | 清华大学 | For the extra specific surface area perovskite type composite oxide catalyst of hydrocarbon low-temperature oxidation and its preparation |
| CN109224761A (en) * | 2017-11-09 | 2019-01-18 | 新昌县以琳环保科技有限公司 | The technique of VOCs treatment containing chlorine |
| CN108837823A (en) * | 2018-06-15 | 2018-11-20 | 万华化学集团股份有限公司 | A kind of perovskite type catalyst and its monoblock type forming method and application |
| CN109157977A (en) * | 2018-09-26 | 2019-01-08 | 中国科学院大学 | A kind of method and catalyst handling volatility chlorinated aromatic hydrocarbons pollutant |
| CN112337461A (en) * | 2020-10-26 | 2021-02-09 | 苏州大学 | Composite material of strontium-doped ordered mesoporous lanthanum manganate-loaded noble metal palladium, preparation method thereof and application thereof in catalytic oxidation of toluene |
| CN112337461B (en) * | 2020-10-26 | 2023-11-03 | 苏州大学 | Composite material of strontium doped ordered mesoporous lanthanum manganate loaded with noble metal palladium, preparation method thereof and application thereof in catalytic oxidation of toluene |
| CN114768836A (en) * | 2022-04-19 | 2022-07-22 | 浙江师范大学 | Catalyst for catalytic oxidation of dichloromethane and preparation method thereof |
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Application publication date: 20140806 |