CN107670658A - Catalyst for chlorobenzene low-temperature catalytic burning and its preparation method and application - Google Patents
Catalyst for chlorobenzene low-temperature catalytic burning and its preparation method and application Download PDFInfo
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
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- B01J23/002—Mixed oxides other than spinels, e.g. perovskite
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/56—Platinum group metals
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- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/0201—Impregnation
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- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
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- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/082—Decomposition and pyrolysis
- B01J37/088—Decomposition of a metal salt
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- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/10—Heat treatment in the presence of water, e.g. steam
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23G—CREMATION FURNACES; CONSUMING WASTE PRODUCTS BY COMBUSTION
- F23G7/00—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals
- F23G7/06—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases
- F23G7/07—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases in which combustion takes place in the presence of catalytic material
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Abstract
The invention discloses the TiO that a kind of catalyst for chlorobenzene low-temperature catalytic burning and its preparation method and application, the catalyst are mainly adulterated by Ce2Formed as carrier and its ruthenium-oxide or vanadium oxide of load, wherein Ce and Ti atomic ratio are 2:8~4:6, with oxide RuO2Or V2O5Account for vehicle weight percentage meter, RuO2Or V2O5Load capacity be 0.5% ~ 2%.Carrier is prepared using the method for solvent volatilization self assembly, and active component is introduced by infusion process.The method for preparing catalyst is simple, does not produce waste liquid, and catalyst of the present invention is burnt the features such as active high, accessory substance is few and stability is good for chlorobenzene catalysis, and chloro volatile organic matter is eliminated especially suitable for low-temperature catalytic burning.
Description
Technical field
The invention belongs to be catalyzed environmental technology field, more particularly to a kind of catalyst for chlorobenzene low-temperature catalytic burning and
Its preparation method and application.
Background technology
Chloride VOC CVOCs（Chlorinated Volatile Organic Compounds）With
Many host materials are compatible, and industrially tool has been widely used, and is one kind in VOCs.Wherein chlorinated aromatic hydrocarbons pollute
Thing is mostly come from industrial processes leakage and discharge and city garbage burning or thermal power plant's waste gas, and its chemical property is steady
It is fixed, it can accumulate in vivo, harm is very big.Main harm includes suppressing nerve center, damages liver and kidney.Due to above-mentioned
The process for producing pollutant is involved in the industry of national economy at this stage, and the discharge of a large amount of chlorine-containing compounds is inevitable
's.Therefore, do not possess the possibility of pollution caused by elimination chlorine-containing volatile hydro carbons from source also at present.And locate after taking
The method of reason eliminates one of chlorinated aromatic hydrocarbon pollutant most efficient method.
In recent years, the comprehensive regulation for VOC (VOCs) received more and more extensive pass
Note.At present, for the removal of chloride volatile organic matter, mainly physical method and the major class technology of chemical method two are included.Physics
Method mainly includes：Activated adoption method, absorb scavenging, condensation collecting method and bioremediation.Chemical method mainly includes：
Catalytic hydrogenation and dechlorination method, photocatalytic degradation method and Production by Catalytic Combustion Process.Wherein Production by Catalytic Combustion Process is used as oxidation using the oxygen in air
Agent, CVOCs completely burneds at a certain temperature, transforms into H2O、CO2, HCl and Cl2Deng product.Catalysis burning possesses
Operation temperature low (250oC-550 oC low concentration pollutant, product (CO), can effectively be eliminated2, HCl and H2O choosing)
Selecting property height,
The features such as more chloro accessory substances are selectively low, it is considered to be eliminate the most economical effective technologies of CVOCs.
Catalyst currently used for chloro volatile organic compounds by catalytic combustion mainly includes three major types：Carried noble metal is urged
Agent, solid acid catalyst and metal oxide catalyst.It is used for the representative patents document of chlorohydrocarbon catalysis burning in recent years
There are JP201410161656, JP201410605598, JP201180042760, JP 2001327869, JP
10085559A2U.S.Patent 4031149、U.S.Patent4059677、U.S.Patent4065543、U.S.Patent
4561969th, U.S.Patent 5811628, U.S.Patent 4169862, U.S.Patent7052663 etc..For chloro virtue
The catalyst of fragrant hydrocarbon low-temperature catalytic burning mainly has V2O5- Ti catalyst, CeO2-TiO2Catalyst, TiO2The Fe of modification3O4Catalysis
The catalyst such as agent.Wherein V bases catalyst activity and stability are preferable, but vanadic anhydride is carcinogen, largely using pole
Easily cause secondary pollution.Therefore the present invention discloses a kind of TiO adulterated with Ce2Ruthenium-oxide or oxidation as carrier and its load
The loaded catalyst that vanadium is formed, composite oxide catalysts dosage pole of the content compared to current V of vanadium in the catalyst
It is low, greatly reduce secondary pollution.And catalyst uses the TiO of cerium dopping in the present invention2As carrier, the two acts synergistically,
So that the carrier has higher stability and surface oxygen mobility simultaneously.Obtained with the carrier loaded ruthenium-oxide or vanadium oxide
Catalyst for chlorobenzene catalysis burning it is active high, accessory substance is few and stability is good the features such as, urged especially suitable for low temperature
Change burning and eliminate chloro volatile organic matter.
The content of the invention
In order to overcome the shortcomings of the prior art, present invention aims at：One kind is provided and is used for the low-temperature catalyzed combustion of chlorobenzene
The catalyst of burning.
Still a further object of the present invention is：A kind of preparation method of above-mentioned catalyst prod is provided.
Still a further object of the present invention is：A kind of application of the said goods is provided.
The object of the invention is realized by following proposal：A kind of catalyst for chlorobenzene low-temperature catalytic burning, the catalyst
It is the TiO adulterated with Ce2Formed as carrier and its ruthenium-oxide or vanadium oxide of load, wherein Ce and Ti atomic ratio are 2:8~
4:6, with oxide RuO2Or V2O5Account for the percent by weight of carrier, RuO2Or V2O5Load capacity be 0.5% ~ 2%.
The present invention provides a kind of preparation method for chlorobenzene low-temperature catalytic burning catalyst, comprises the following steps：
（1）The preparation of carrier
The first step：Using six nitric hydrate ceriums as cerium precursor, 0.25mol/L cerous nitrate ethanol solution is prepared；
Second step：Presoma using isopropyl titanate as titanium, prepare 0.25mol/L isopropyl titanate ethanol solution；
3rd step：Atomic ratio according to Ce and Ti is 2:8~4:6, measure the cerous nitrate ethanol solution and isopropyl titanate of certain volume
Ethanol solution；
4th step：Water-bath is placed in fume hood, 40 ~ 60oUnder conditions of C water-baths, cerous nitrate ethanol solution is added dropwise
Enter into isopropyl titanate ethanol solution；
5th step：Calculating added isopropyl titanate hydrolysis needs the amount of water, according to the amount of the crystallization water contained by six nitric hydrate ceriums,
Calculate isopropyl titanate hydrolysis and require supplementation with the amount for adding water, be added dropwise according to the amount of the water calculated into mixed aqueous solution
The amount of ionized water；
6th step：By above-mentioned mixed solution under conditions of water-bath, stirring is until faint yellow viscous pasty state in ventilating kitchen；
7th step：By obtained gum-like product in 60oC~80oIt is dried overnight under the conditions of C, in 500oC~600o2 ~ 4h is calcined under C to obtain
To the TiO of Ce doping2Carrier；
（2）The preparation of loaded catalyst
The first step：The TiO of different ratio Ce doping is measured respectively2The water absorption rate of carrier, configured according to the water absorption rate of carrier different
The chlorination ruthenium solution and ammonium metavanadate solution of concentration；
Second step：Chlorination ruthenium solution and ammonium metavanadate solution are loaded on carrier respectively using equi-volume impregnating；
3rd step：By obtained presoma in 80oC~120oIt is dried overnight under the conditions of C, in 400oC~500o2 ~ 4h is calcined under C, is obtained
To prepared cerium-titanium composite oxide-carried ruthenium-oxide and vanadium oxide catalyst.
Catalyst of the present invention is prepared using the method for solvent volatilization self assembly, it is not necessary to and filter, do not produce waste liquid, and
The catalyst granules of preparation is uniform, and minimal amount of RuO is introduced on carrier2Or V2O5, on the one hand can improve the work of catalyst
Property, the production of more chloro accessory substances on the other hand can be reduced, the catalysis burning for chlorohydrocarbon has great importance.
The present invention provides a kind of catalyst and is used for the application that chlorobenzene low-temperature catalytic burning eliminates.
Catalyst of the present invention has following features：
（1）The present invention using the titanium dioxide of cerium dopping as carrier, cerium doped titanium dioxide make carrier produce surface defect so that
The mobility of oxygen is improved, and then improves catalyst activity；
（2）The titanium dioxide of cerium dopping can suppress surface chlorion and active oxygen and surface during catalyst reaction
The exchange of hydroxyl, so as to improve stability；
（3）Catalyst is loaded on carrier using minimal amount of vanadium in the present invention, compare traditional catalyst greatly reduce it is secondary
Pollution, has very high Practical significance.
Specific embodiment
Embodiment 1
Weigh the nitric hydrate ceriums of 1.73g six to be dissolved in 40ml ethanol, stir, form six nitric hydrate cerium alcoholic solutions, be designated as
Solution A；The isopropyl titanate for weighing 4.55g 98% is dissolved in 40ml ethanol, is stirred, and it is molten to form uniform isopropyl titanate ethanol
Liquid, it is designated as solution B.In fume hood, 40oUnder conditions of C water-baths, solution A is added drop-wise in B solution dropwise, it is to be mixed uniform
Afterwards, 1g deionized waters are continuously added into above-mentioned mixed solution, continues stirring to clear yellow viscous colloidal mixture is formed, will be formed
Mixture be placed in 100oIt is dried overnight in C baking ovens, taking-up is placed in Muffle furnace in 500 after grindingo3h is calcined under the conditions of C, is obtained
Ce0.2Ti0.8O2。
Embodiment 2
Weigh the nitric hydrate ceriums of 2.60g six to be dissolved in 40ml ethanol, stir, form six nitric hydrate cerium alcoholic solutions, be designated as
Solution A；The isopropyl titanate for weighing 4.06g 98% is dissolved in 40ml ethanol, is stirred, and it is molten to form uniform isopropyl titanate ethanol
Liquid, it is designated as solution B.In fume hood, 40oUnder conditions of C water-baths, solution A is added drop-wise in B solution dropwise, it is to be mixed uniform
Afterwards, 1g deionized waters are continuously added into above-mentioned mixed solution, continues stirring to clear yellow viscous colloidal mixture is formed, will be formed
Mixture be placed in 100oIt is dried overnight in C baking ovens, taking-up is placed in Muffle furnace in 500 after grindingo3h is calcined under the conditions of C, is obtained
Ce0.3Ti0.7O2。
Embodiment 3
Weigh the nitric hydrate ceriums of 3.47g six to be dissolved in 40ml ethanol, stir, form six nitric hydrate cerium alcoholic solutions, be designated as
Solution A；The isopropyl titanate for weighing 3.41g 98% is dissolved in 40ml ethanol, is stirred, and it is molten to form uniform isopropyl titanate ethanol
Liquid, it is designated as solution B.In fume hood, 40oUnder conditions of C water-baths, solution A is added drop-wise in B solution dropwise, it is to be mixed uniform
Afterwards, 1g deionized waters are continuously added into above-mentioned mixed solution, continues stirring to clear yellow viscous colloidal mixture is formed, will be formed
Mixture be placed in 100oIt is dried overnight in C baking ovens, taking-up is placed in Muffle furnace in 500 after grindingo3h is calcined under the conditions of C, is obtained
Ce0.4Ti0.6O2。
Embodiment 4
Weigh the Ce of the preparation of 1g embodiments 10.2Ti0.8O2Carrier, measurement water absorption rate are 120%；0.80g ammonium metavanadates are weighed to be dissolved in
In 150 ml deionized waters, 0.0450mol/L ammonium metavanadate solution is prepared；Weigh what is prepared in 1g embodiments 1
Ce0.2Ti0.8O2Carrier, measures 1.2 milliliters of above-mentioned ammonium metavanadate standard liquids, and ammonium metavanadate is impregnated into load using equi-volume impregnating
On body.In 60 oCIt is dried overnight in baking oven, in 550oC Muffle kiln roasting 4h, obtain 0.5%V2O5-Ce0.2Ti0.8O2Catalyst.
Embodiment 5
Weigh 3.20 ammonium metavanadates to be dissolved in 150 ml deionized waters, prepare 0.1350mol/L ammonium metavanadate solution；Weigh
The Ce prepared in 1g embodiments 10.3Ti0.7O2Carrier, 1.2 milliliters of above-mentioned ammonium metavanadate standard liquids are measured, using equi-volume impregnating
Ammonium metavanadate is impregnated on carrier.In 70 oCIt is dried overnight in baking oven, in 600oC Muffle kiln roasting 2h, obtain 2.0%
V2O5- Ce0.3Ti0.7O2Catalyst.
Embodiment 6
Weigh the hydrate ruthenium trichlorides of 2.40g tri- to be dissolved in 150 ml deionized waters, prepare 0.06mol/L solution of ruthenium trichloride,
Weigh the Ce of the preparation of 1g embodiments 30.4Ti0.6O2Carrier, 1.2 milliliters of above-mentioned ruthenium trichloride standard liquids are measured, using incipient impregnation
Ruthenium trichloride standard liquid is impregnated on carrier by method.In 80oIt is dried overnight in C baking ovens, in 550oC Muffle kiln roasting 4h, are obtained
1.0%RuO2- Ce0.4Ti0.6O2Catalyst.
Catalyst activity is evaluated
Used catalyst activity rating for chlorobenzene catalysis burning is in fixed-bed micro-reactor（Internal diameter 3mm quartz）Middle progress,
The dosage of catalyst is 200mg, and temperature is automatically controlled using K type thermocouples.Using 100 systems of Stoelting companies of the U.S.
Chlorobenzene injection is entered vaporizer by row KDS120 types micro-injection pump, and being then mixed into reactor with air is burnt.Always
Flow is controlled using mass flowmenter, and the concentration of chlorobenzene is 0.1vol%, and the exhausted air quantity that every gram of catalyst is handled per hour is 15L,
The linear velocity of the gas of reacted device is 100m/h, reaction pressure 0.1MPa.The conversion ratio of chlorobenzene and the relation of reaction temperature
It is shown in Table 1, T in table50、T90Respectively conversion ratio reaches reaction temperature required when 50%, 90%.Reaction end gas is through chromatogram and matter
The online tracking of spectrum, key reaction product is carbon dioxide, hydrogen chloride and a small amount of chlorine.
From the results shown in Table 1, removal of the catalyst of the preparation of the method for chlorobenzene has preferably catalysis
Performance, and the method for preparing catalyst is simple, can efficiently reduce the generation of accessory substance after introducing Ru or V into catalyst, because
This catalyst has very high practical value.
Claims (3)
1. a kind of catalyst for chlorobenzene low-temperature catalytic burning, it is characterised in that the catalyst is the TiO adulterated with Ce2As
Carrier and its ruthenium-oxide or vanadium oxide of load are formed, and wherein Ce and Ti atomic ratio are 2:8~4:6, with oxide RuO2Or
V2O5Account for the percent by weight of carrier, RuO2Or V2O5Load capacity be 0.5% ~ 2%.
A kind of 2. preparation method according to claim 1 for chlorobenzene low-temperature catalytic burning catalyst, it is characterised in that
Specifically include following steps：
（1）The preparation of carrier
The first step：Using six nitric hydrate ceriums as cerium precursor, 0.25mol/L cerous nitrate ethanol solution is prepared；
Second step：Presoma using isopropyl titanate as titanium, prepare 0.25mol/L isopropyl titanate ethanol solution；
3rd step：Atomic ratio according to Ce and Ti is 2:8~4:6, measure the cerous nitrate ethanol solution and isopropyl titanate of certain volume
Ethanol solution；
4th step：Water-bath is placed in fume hood, 40 ~ 60oUnder conditions of C water-baths, cerous nitrate ethanol solution is added dropwise
Into isopropyl titanate ethanol solution；
5th step：Calculating added isopropyl titanate hydrolysis needs the amount of water, according to the amount of the crystallization water contained by six nitric hydrate ceriums,
Calculate isopropyl titanate hydrolysis and require supplementation with the amount for adding water, be added dropwise according to the amount of the water calculated into mixed aqueous solution
The amount of ionized water；
6th step：By above-mentioned mixed solution under conditions of water-bath, stirring is until faint yellow viscous pasty state in ventilating kitchen；
7th step：By obtained gum-like product in 60oC~80oIt is dried overnight under the conditions of C, in 500oC~600o2 ~ 4h is calcined under C to obtain
To the TiO of Ce doping2Carrier；
（2）The preparation of loaded catalyst
The first step：The TiO of different ratio Ce doping is measured respectively2The water absorption rate of carrier, configured according to the water absorption rate of carrier different dense
The chlorination ruthenium solution and ammonium metavanadate solution of degree；
Second step：Chlorination ruthenium solution and ammonium metavanadate solution are loaded on carrier respectively using equi-volume impregnating；
3rd step：By obtained presoma in 80oC~120oIt is dried overnight under the conditions of C, in 400oC~500o2 ~ 4h is calcined under C, is obtained
To prepared cerium-titanium composite oxide-carried ruthenium-oxide and vanadium oxide catalyst.
3. catalyst is used for the application that chlorobenzene low-temperature catalytic burning eliminates according to claim 1.
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| CN110102292A (en) * | 2019-04-09 | 2019-08-09 | 中国船舶重工集团公司第七一八研究所 | A kind of preparation method for eliminating chlorine-containing organic compounds exhaust gas catalyst |
| WO2021000672A1 (en) * | 2019-07-03 | 2021-01-07 | 浙江大学 | High-efficiency anti-chlorine poisoning catalyst for catalytic oxidation of volatile organic compound and preparation method therefor |
| CN113786828A (en) * | 2021-09-16 | 2021-12-14 | 清华大学 | Catalyst for synergistic removal of NOx and CVOCs and preparation method and application thereof |
| CN114272923A (en) * | 2022-01-06 | 2022-04-05 | 浙江大学 | Chlorine-resistant water-resistant catalyst and preparation method and application thereof |
| CN114289018A (en) * | 2021-11-25 | 2022-04-08 | 上海环境卫生工程设计院有限公司 | High HCl selectivity chlorine-containing organic matter combustion catalyst and preparation method thereof |
| CN114602458A (en) * | 2022-03-22 | 2022-06-10 | 江苏理工学院 | Mn (VO)3)2/V2O5Catalyst, preparation method and application thereof |
| CN115400745A (en) * | 2022-07-28 | 2022-11-29 | 常州大学 | Cerium-based catalyst for efficiently degrading CVOCs (chemical vapor deposition) |
| CN115722220A (en) * | 2022-12-08 | 2023-03-03 | 郑州大学 | Catalytic oxidation catalyst, and preparation method and application thereof |
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Cited By (12)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN110102292A (en) * | 2019-04-09 | 2019-08-09 | 中国船舶重工集团公司第七一八研究所 | A kind of preparation method for eliminating chlorine-containing organic compounds exhaust gas catalyst |
| WO2021000672A1 (en) * | 2019-07-03 | 2021-01-07 | 浙江大学 | High-efficiency anti-chlorine poisoning catalyst for catalytic oxidation of volatile organic compound and preparation method therefor |
| CN113786828A (en) * | 2021-09-16 | 2021-12-14 | 清华大学 | Catalyst for synergistic removal of NOx and CVOCs and preparation method and application thereof |
| CN113786828B (en) * | 2021-09-16 | 2023-12-29 | 清华大学 | Catalyst for synergistic removal of NOx and CVOCs, and preparation method and application thereof |
| CN114289018A (en) * | 2021-11-25 | 2022-04-08 | 上海环境卫生工程设计院有限公司 | High HCl selectivity chlorine-containing organic matter combustion catalyst and preparation method thereof |
| CN114272923A (en) * | 2022-01-06 | 2022-04-05 | 浙江大学 | Chlorine-resistant water-resistant catalyst and preparation method and application thereof |
| CN114272923B (en) * | 2022-01-06 | 2023-10-31 | 浙江大学 | Chlorine-resistant water-resistant catalyst and preparation method and application thereof |
| CN114602458A (en) * | 2022-03-22 | 2022-06-10 | 江苏理工学院 | Mn (VO)3)2/V2O5Catalyst, preparation method and application thereof |
| CN114602458B (en) * | 2022-03-22 | 2023-05-26 | 江苏理工学院 | Mn (VO 3 ) 2 /V 2 O 5 Catalyst, preparation method and application thereof |
| CN115400745A (en) * | 2022-07-28 | 2022-11-29 | 常州大学 | Cerium-based catalyst for efficiently degrading CVOCs (chemical vapor deposition) |
| CN115722220A (en) * | 2022-12-08 | 2023-03-03 | 郑州大学 | Catalytic oxidation catalyst, and preparation method and application thereof |
| CN115722220B (en) * | 2022-12-08 | 2024-04-02 | 郑州大学 | Catalytic oxidation catalyst and preparation method and application thereof |
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