CN101874980A - Application of transition-metal substituted type hexaaluminate high-temperature catalytic material in enameled-wire waste gas treatment - Google Patents
Application of transition-metal substituted type hexaaluminate high-temperature catalytic material in enameled-wire waste gas treatment Download PDFInfo
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- CN101874980A CN101874980A CN 201010154883 CN201010154883A CN101874980A CN 101874980 A CN101874980 A CN 101874980A CN 201010154883 CN201010154883 CN 201010154883 CN 201010154883 A CN201010154883 A CN 201010154883A CN 101874980 A CN101874980 A CN 101874980A
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Abstract
The invention relates to application of a high-activity high-stability transition-metal substituted type hexaaluminate catalyst in high-concentration volatile organic waste gas catalytic oxidation of an enameled wire industry. The expression formula of the catalyst is BaxLa1-xRyR'zAl12-y-zO19- delta, wherein R and R' are respectively crystal lattice substituted components of Mn, Ti, Fe, Co, Zr, Ni, Cu and the like. The catalyst has simple preparation process and good stability, and the specific surface area of the material after 1100 DEG C/3h high-temperature roasting can still reach 40-60m<2>/g; researches indicate that all the organic waste gases can be completely converted into CO2 and H2O by the catalyst at the temperature of 700 DEG C under the conditions of different airspeeds (30,000-90,000h-1), different pollutant concentrations (1000-5000mg/m<3>) and different relative humidifies (0-70% RH). Meanwhile, the catalyst is safe and stable in high-temperature operation and is not inactivated through hydrothermal stability inspection for 300 hours. Integrated type catalysts with different structures can be obtained by coating the prepared substituted type hexaaluminate material as an active component on an integrated type ceramic surface, and the substituted type hexaaluminate material can be applied to the organic waste gas treatment of the enameled wire industry and has good application potential.
Description
Technical field
The present invention relates to high activity, the application of high stability transition-metal substituted type hexa-aluminate catalysis material in enamel-covered wire high concentration volatile organic matter (dimethylbenzene, ethylbenzene and phenyl methylcarbamate) catalytic oxidation.
Background technology
Enamel-covered wire is the critical material of motor, electrical equipment, electronic instrument etc., after the China's entry into the WTO, the Chinese lacquer envelope curve enters a new high speed development stage, the enamel-covered wire volume of production and marketing from nineteen ninety account for 6.2% of global total output bring up to 2000 15.4%, 2005 near 30%, expect 2015 and will bring up to about 50%, become Production of Enamel Wires worthy of the name and sell big country.Employed lacquer liquid is made by synthetic resin and solvent in the Production of Enamel Wires process, and wherein solvent accounts for 70%, is mainly dimethylbenzene, ethylbenzene and phenyl methylcarbamate, and such organic solvent evaporates into (concentration＞2000mg/m in the atmosphere in a large number at bake process
3).The high concentration volatile organic matter can cause a lot of harmful environmental effects on the one hand, as photochemical fog; Its harm to human body also can not be ignored on the other hand, and the short-term suction can make symptoms such as the people clouding of consciousness, headache occurs, feels sick, vomiting, muscle cramp; Long-term contact can make human body anaemia occur, even canceration takes place.
Carried noble metal (Pd, Pt, Ag etc.) catalyst has good low temperature active, but it costs an arm and a leg, and active component is volatile, sintering and poisoning.Catalyst of transition metal oxide with low cost, warm catalytic oxidation in being mainly used in, yet its anti-poison and sintering character relatively poor.Common oxide and perovskite structure composite oxide catalyst exist the easy-sintering inactivation equally.
Hexa-aluminate class catalyst is described as the high-temp combustion of application prospect catalyst most, and its outstanding advantage is that it has β-Al
2O
3Or the unique layer structure of Magnetoplumbate-type, Stability Analysis of Structures still can be kept higher specific surface area when temperature is higher than 1200 ℃, have good anti-sintering and thermal shock resistance properties in catalytic reaction.The general formula of hexa-aluminate is AAl
12O
19, the A position ion in its lattice and the Al of B position
3+Ion can be replaced by the close metal ion of radius, generates the better metal substituted type of catalytic activity hexa-aluminate catalyzer.
We are granted patent (publication number: CN 1680020A) adopt different preparation methods to obtain the hexa-aluminate catalyzer of the Transition metal substituted of high-specific surface area, high stability.On this basis, we are applied to the transition-metal substituted type hexa-aluminate catalyzer that obtains the catalytic oxidation of enamel-covered wire high concentration VOCs waste gas.Simultaneously, prepared hexa-aluminate high-temperature catalytic material is coated in the monoblock type ceramic surface as active phase constituent, obtains the integral catalyzer of different structure, can be applied to enamel-covered wire industry organic exhaust gas and handle, have good application prospects.
Summary of the invention
The objective of the invention is the transition-metal substituted type hexa-aluminate catalyzer is applied to the catalytic oxidation of enamel-covered wire high concentration volatility organic contamination waste gas (VOCs), provide that a kind of preparation technology is simple, high catalytic activity, long-time running are stable, the catalysis material of economic environmental protection.
For achieving the above object, the present invention gives full play to hexa-aluminate and transition metal (Mn, Ti, Fe, Co, Zr, Ni, Cu etc.) separately advantage, greatly improve the catalytic activity and the hydrothermal stability of catalyst, high concentration, high-speed dimethylbenzene, ethylbenzene, the phenyl methylcarbamate complete oxidation that the enamel-covered wire industry can be produced are CO
2And H
2O reaches economic environmental protection, stable purpose.Wherein:
VOCs mainly wraps dimethylbenzene, ethylbenzene and phenyl methylcarbamate;
VOCs concentration is 1000-5000mg/m
3
Reaction velocity is 30,000-90,000h
-1(air speed is 110 on the integral catalyzer, 000h
-1);
The reactant water content is 0-70%RH;
Reaction temperature is 130-700 ℃.
Simultaneously, prepared hexa-aluminate high-temperature catalytic material is coated in the monoblock type ceramic surface as active component, obtains the integral catalyzer of different structure, can be applied to enamel-covered wire industry organic exhaust gas and handle, have great application prospect.
The present invention is the transition-metal substituted type hexa-aluminate catalyzer, is mainly used in the catalytic oxidation of enamel-covered wire industry middle and high concentration dimethylbenzene, ethylbenzene, phenyl methylcarbamate, and expects that this catalysis material can be applied to the catalytic purification of other relevant industries VOCs.
Description of drawings
Fig. 1 is Ba among the present invention
0.2La
0.8FeMnAl
10O
19(1100 ℃/3h) pore distribution curve (A) and N of catalyst
2Adsorption desorption curve (B);
Fig. 2 is Ba among the present invention
0.2La
0.8FeMnAl
10O
19(1100 ℃/3h) SEM photo of catalyst;
Fig. 3 is Ba among the present invention
0.2La
0.8FeMnAl
10O
19Catalyst (1100 ℃/3h) to the conversion rate curve of variable concentrations dimethylbenzene, ethylbenzene and phenyl methylcarbamate (air speed: 30,000h
-1);
Fig. 4 is Ba among the present invention
0.2La
0.8FeMnAl
10O
19Catalyst (1100 ℃/3h) to the conversion rate curve (pollutant levels: 3000mg/m of dimethylbenzene, ethylbenzene and phenyl methylcarbamate under the different air speeds
3);
Fig. 5 is Ba among the present invention
0.2La
0.8FeMnAl
10O
19Catalyst (1100 ℃/3h) to the conversion rate curve (pollutant levels: 3000mg/m of dimethylbenzene, ethylbenzene and phenyl methylcarbamate under the different relative humidity
3, air speed: 30,000h
-1);
Fig. 6 is Ba among the present invention
0.2La
0.8FeMnAl
10O
19(1100 ℃/3h) stability test (pollutant levels: 3000mg/m of catalyst
3, air speed: 30,000h
-1, relative humidity: 30%RH, reaction temperature be 300 ℃).
The specific embodiment
The preparation method of transition-metal substituted type hexa-aluminate catalysis material is as described in the patent CN 1680020A.Gas generating unit is three gas circuit VOCs generators in the experiment, and catalytic oxidation carries out on continuous flow reactor of fixed bed.Investigated the catalytic oxidation stable and paraxylene, ethylbenzene and phenyl methylcarbamate under different pollutant levels, different air speed and different moisture content condition of transition-metal substituted type hexa-aluminate catalyzer.Studies show that, under the differential responses condition, typical transition-metal substituted type hexa-aluminate catalysis material (Ba
0.2La
0.8FeMnAl
10O
19) can be in 700 ℃ be eco-friendly CO with the complete catalytic oxidation of the mix waste gas of dimethylbenzene, ethylbenzene and phenyl methylcarbamate
2And H
2O; Simultaneously, catalyst is investigated through the 300h hydrothermal stability, inactivation do not occur.
Embodiment 1Ba
0.2La
0.8FeMnAl
10O
19Catalytic oxidation to variable concentrations dimethylbenzene, ethylbenzene and phenyl methylcarbamate
Adopt fixed bed continuous-flow reaction evaluating device, take by weighing 500mg Ba
0.2La
0.8FeMnAl
10O
19Catalyst places in the stainless steel reaction pipe (internal diameter 6mm), regulates the carrier gas flux of dimethylbenzene, ethylbenzene and phenyl methylcarbamate place gas circuit respectively, and making separately, concentration reaches 1000mg/m respectively
3, 3000mg/m
3And 5000mg/m
3The air mixed gas flow is about 300mlmin in the reaction
-1, make reaction velocity reach 30,000h
-1The result shows, Ba
0.2La
0.8FeMnAl
10O
19Catalyst can be in 550 ℃ is CO with dimethylbenzene, ethylbenzene and the phenyl methylcarbamate complete oxidation of variable concentrations
2And H
2O.
Embodiment 2Ba
0.2La
0.8FeMnAl
10O
19Catalytic oxidation to dimethylbenzene, ethylbenzene and phenyl methylcarbamate under the different air speeds
Adopt fixed bed continuous-flow reaction evaluating device, take by weighing 500mg Ba
0.2La
0.8FeMnAl
10O
19Catalyst places in the stainless steel reaction pipe (internal diameter 6mm), is 300-900mlmin with the air Mixture flow-control
-1, regulate the carrier gas flux of dimethylbenzene, ethylbenzene and phenyl methylcarbamate place gas circuit respectively, make its concentration reach 3000mg/m respectively
3Reaction velocity is controlled to be 30 respectively, 000h
-1, 60,000h
-1With 90,000h
-1The result shows, Ba
0.2La
0.8FeMnAl
10O
19Catalyst under different air speed conditions, can be in 700 ℃ be CO with dimethylbenzene, ethylbenzene and phenyl methylcarbamate complete oxidation
2And H
2O.
Embodiment 3Ba
0.2La
0.8FeMnAl
10O
19Catalytic oxidation to dimethylbenzene, ethylbenzene and phenyl methylcarbamate under the different relative humidity
Adopt fixed bed continuous-flow reaction evaluating device, take by weighing 500mg Ba
0.2La
0.8FeMnAl
10O
19Catalyst places in the stainless steel reaction pipe (internal diameter 6mm), is 300mlmin with the air Mixture flow-control
-1, regulate the carrier gas flux of dimethylbenzene, ethylbenzene and phenyl methylcarbamate place gas circuit respectively, make its concentration reach 3000mg/m respectively
3, reaction velocity is controlled to be 30,000h
-1, the control reaction humidity is 30%RH and 70%RH.The result shows, Ba
0.2La
0.8FeMnAl
10O
19Catalyst under the different humidity condition, can be in 650 ℃ be CO with dimethylbenzene, ethylbenzene and phenyl methylcarbamate complete oxidation
2And H
2O.
Embodiment 4Ba
0.2La
0.8FeMnAl
10O
19The study on the stability of material
Adopt fixed bed continuous-flow reaction evaluating device, take by weighing 500mg Ba
0.2La
0.8FeMnAl
10O
19Catalyst places in the stainless steel reaction pipe (internal diameter 6mm), is 300mlmin with the air Mixture flow-control
-1, regulate the carrier gas flux of dimethylbenzene, ethylbenzene and phenyl methylcarbamate place gas circuit respectively, make its concentration reach 3000mg/m respectively
3, reaction humidity is 30%RH, reaction velocity is controlled to be 30,000h
-1, reaction temperature is 300 ℃.Through 300h stability test, Ba
0.2La
0.8FeMnAl
10O
19Obvious inactivation does not appear in catalyst.
The preparation of embodiment 5 monoblock type hexa-aluminate catalyzers is with active
Above Transition metal substituted hexa-aluminate catalyzer material is coated in the monoblock type ceramic surface as active component, can obtains the integral catalyzer of different honeycombs.
Experiment is measured the catalytic oxidation activity of integral catalyzer, and it is in the reaction tube of 16mm that integral catalyzer places internal diameter, and the composition of organic pollution is identical with above-mentioned experiment, and concentration is 3000mg/m
3, reaction humidity is 30%RH, reaction velocity is 110,000h
-1The result shows that catalyst can be with the complete catalytic oxidation of above-mentioned waste gas in 700 ℃.
Claims (4)
1. the application of transition-metal substituted type hexa-aluminate high-temperature catalytic material in enamel-covered wire high concentration volatile organic matter (VOCs) catalytic oxidation.
2. employed transition-metal substituted type hexa-aluminate high-temperature catalytic material be based upon we granted patent (publication number: CN1680020A) obtain on the basis, the present invention is primarily aimed at the application of such material in enamel-covered wire industry high-concentration organic waste gas.
3. according to claim 1, the transition-metal substituted type hexa-aluminate catalyzer is mainly used in the catalytic oxidation of enamel-covered wire industry high concentration VOCs among the present invention, wherein:
VOCs mainly wraps dimethylbenzene, ethylbenzene and phenyl methylcarbamate;
VOCs concentration is 1000-5000mg/m
3
Gas space velocity is 30,000-90,000h
-1(air speed is 110 on the integral catalyzer, 000h
-1);
The reactant water content is 0-70%RH;
Reaction temperature is 130-700 ℃.
4. as transition-metal substituted type hexa-aluminate catalyzer as described in the claim 2, it is coated in the monoblock type ceramic surface as active component, can obtains the integral catalyzer of different structure, can be applied to enamel-covered wire industry organic exhaust gas and handle.
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|---|---|---|---|
| CN201010154883.3A CN101874980B (en) | 2010-04-26 | 2010-04-26 | Application of transition-metal substituted type hexaaluminate high-temperature catalytic material in enameled-wire waste gas treatment |
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|---|---|---|---|
| CN201010154883.3A CN101874980B (en) | 2010-04-26 | 2010-04-26 | Application of transition-metal substituted type hexaaluminate high-temperature catalytic material in enameled-wire waste gas treatment |
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| CN101874980B CN101874980B (en) | 2014-03-26 |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2016062853A1 (en) * | 2014-10-24 | 2016-04-28 | Basf Se | High-temperature synthesis of aluminates by flame spray pyrolysis |
| CN114811624A (en) * | 2021-01-22 | 2022-07-29 | 中国科学院大学 | DMF-containing waste gas purification and collaborative production N 2 Method of O |
| CN116899249A (en) * | 2023-09-13 | 2023-10-20 | 山西诚宏福得一化工有限公司 | Light benzene separation processing device and processing technology thereof |
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| JPH06226099A (en) * | 1993-01-29 | 1994-08-16 | Osaka Gas Co Ltd | Composite catalyst body for high-temperature combustion |
| US20040110634A1 (en) * | 2002-12-05 | 2004-06-10 | Labarge William J. | PROX catalyst for oxidizing carbon monoxide |
| CN1680020A (en) * | 2004-04-05 | 2005-10-12 | 中国科学院生态环境研究中心 | Preparation of transition metal substituted hexaaluminate as catalyst for natural gas combustion |
| JP2006239650A (en) * | 2005-03-07 | 2006-09-14 | Denki Kagaku Kogyo Kk | Catalyst carrier and its production method |
| CN101306361A (en) * | 2007-05-15 | 2008-11-19 | 北京石油化工学院 | Method for preparing hexa-aluminate catalyst using reversed phase micro-emulsion method |
| CN101612572A (en) * | 2008-06-26 | 2009-12-30 | 北京石油化工学院 | A kind of decomposing N that is used for 2The hexa-aluminate catalyzer of O |
-
2010
- 2010-04-26 CN CN201010154883.3A patent/CN101874980B/en active Active
Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH06226099A (en) * | 1993-01-29 | 1994-08-16 | Osaka Gas Co Ltd | Composite catalyst body for high-temperature combustion |
| US20040110634A1 (en) * | 2002-12-05 | 2004-06-10 | Labarge William J. | PROX catalyst for oxidizing carbon monoxide |
| CN1680020A (en) * | 2004-04-05 | 2005-10-12 | 中国科学院生态环境研究中心 | Preparation of transition metal substituted hexaaluminate as catalyst for natural gas combustion |
| JP2006239650A (en) * | 2005-03-07 | 2006-09-14 | Denki Kagaku Kogyo Kk | Catalyst carrier and its production method |
| CN101306361A (en) * | 2007-05-15 | 2008-11-19 | 北京石油化工学院 | Method for preparing hexa-aluminate catalyst using reversed phase micro-emulsion method |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2016062853A1 (en) * | 2014-10-24 | 2016-04-28 | Basf Se | High-temperature synthesis of aluminates by flame spray pyrolysis |
| CN114811624A (en) * | 2021-01-22 | 2022-07-29 | 中国科学院大学 | DMF-containing waste gas purification and collaborative production N 2 Method of O |
| CN116899249A (en) * | 2023-09-13 | 2023-10-20 | 山西诚宏福得一化工有限公司 | Light benzene separation processing device and processing technology thereof |
| CN116899249B (en) * | 2023-09-13 | 2024-01-02 | 山西诚宏福得一化工有限公司 | Light benzene separation processing device and processing technology thereof |
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| CN101874980B (en) | 2014-03-26 |
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