CN103551141A - Pt/MOx catalyst and application thereof in toluene catalytic combustion - Google Patents

Pt/MOx catalyst and application thereof in toluene catalytic combustion Download PDF

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Publication number
CN103551141A
CN103551141A CN201310459979.4A CN201310459979A CN103551141A CN 103551141 A CN103551141 A CN 103551141A CN 201310459979 A CN201310459979 A CN 201310459979A CN 103551141 A CN103551141 A CN 103551141A
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catalyst
toluene
solution
metal oxide
mox
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严新焕
敖平
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Zhejiang University of Technology ZJUT
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Zhejiang University of Technology ZJUT
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Abstract

The invention discloses a Pt/MOx catalyst and an application thereof in toluene catalytic combustion. The preparation method of the catalyst comprises the steps that: Pt2(dba)3 is added to the propylene glycol carbonate, such that a mixture is obtained; the mixture is subjected to a stirring reaction under room temperature in 1-3MPa hydrogen atmosphere; stirring is stopped after 1-2h, and the solution is fetched, such that a solution comprising Pt nano-particles is obtained; the obtained solution comprising Pt nano-particles is mixed with a metal oxide carrier; magnetic stirring is carried out, such that the Pt nano-particles are completed adhered to the metal oxide carrier; the solution is filtered, and washing and drying are carried out, such that the Pt/MOx catalyst is obtained. The Pt/MOx catalyst provided by the invention can be applied in toluene catalytic combustion. With the synthesis method of the catalyst provided by the invention, waste gas or waste water is not product, and environment cost is low, such that expanded-scale industrialized production can be carried out. The prepared catalyst has high activity and good stability. With the catalyst, low-concentration toluene can be completely oxidized into carbon dioxide and water under low temperature, and no other product is produced.

Description

A kind of Pt/MO xcatalyst and in the aflame application of toluene catalytically
Technical field
The invention belongs to catalyst technical field, be specifically related to a kind of noble metal catalyst Pt/MO xand in the aflame application of toluene catalytically.
Background technology
Toluene is the most common and higher VOCs of concentration of emission in indoor-outdoor air, is mainly derived from the waste gas that discharges in the production processes such as petrochemical industry, Coal Chemical Industry, paint, agricultural chemicals, medicine and the tail gas of waste water and motor vehicle emission.The key component of atmosphere pollution is not only in the release of low concentration VOCs, can form photochemical fog, and is one of main source of PM2.5, and health and ecology are all had to more serious harm, and wherein benzene is known carcinogenic substance.In The Atmosphere Over China pollutant comprehensive discharge standard makes explicit provisions to the highest permission concentration of emission of VOCs, the highest permission rate of discharge and uncontrollable discharge limit value.Therefore effectively remove airborne VOCs very urgent.
Catalytic combustion is to eliminate one of effective and the most the most frequently used method of VOCs.Can reduce reaction temperature on the one hand, and without extraneous heat supply, just can make organic exhaust gas in the lower generation flameless combustion of lower initiation temperature condition (only needing 300 ℃ of left and right) after reaching initiation temperature; On the other hand, can make reactant molecule be enriched in catalyst surface, to improve reaction rate, Quick Oxidation is decomposed into CO 2and H 2o.
In recent years, people have prepared the catalyst of a large amount of catalytic oxidation VOCs gas, comprise noble metal (Pt, Pd, Rh, Au) loaded catalyst and the oxide carried type catalyst of transition metal (Cr, Co, Cu, Ni, Mn).Wherein, the most deep to there is the research of noble metal carrier catalyst (Au, Pt, Pd, Ag) of the features such as high activity and initiation temperature are low, and process in engineering equipment and obtained actual application at VOCs.But the temperature higher (150 ℃-300 ℃) of these their complete oxidation VOCs.The temperature that further reduces VOCs completing combustion has caused numerous researchers' concern and interest, is a focus more always, and therefore urgent need exploitation is a kind of can transform the catalyst of VOCs completely under lower temperature.
The preparation of loaded catalyst is mainly by infusion process, sol-gal process, redox precipitation method, hydro-thermal method etc. at present.These method operations are all more loaded down with trivial details, in the building-up process of catalyst, also can produce a large amount of waste water and waste gas, if understand contaminated environment again without processing directly discharge, and the repeatability of the catalyst prepared of these methods is not good especially, stricter to the operation requirements of preparation process.
Chinese patent CN1415410 has proposed with infusion process by organic acid competitive Adsorption, noble metal active component Pt(is contained to organic acid platiniferous solution) support in honeycomb ceramic carrier coating outer surface, realized the purified treatment that all kinds contain combustible component waste gas at 300 ℃ of temperature.
Chinese patent CN102039198 be take smelling of cationic surfactant cetyl trimethyl amine and is called for short CTAB and non-ionic surface active agent Triton X-100 and by hydro-thermal method, makes catalyst sample for common template, at 270 ℃ by benzene complete oxidation.
The invention provides a kind of high activated catalyst for catalyzed conversion Low Concentration Toluene under lower temperature, this catalyst be take metal oxide as carrier, and on carrier self assembly precious metals pt nano particle.
Summary of the invention
First object of the present invention is to provide that a kind of preparation technology is simple, raw material sources extensively and recoverable, catalytic activity are high, the Pt/MO of good stability xcatalyst.
Second object of the present invention is to provide described Pt/MO xcatalyst is in the aflame application of toluene catalytically, and it can be implemented in catalyzed conversion Low Concentration Toluene under lower temperature.
Below technical scheme of the present invention is illustrated.
The invention provides a kind of Pt/MO xcatalyst, wherein MO xfor metal oxide, its preparation method comprises the steps: Pt 2(dba) 3join and in propylene glycol carbonate, obtain mixture, and this mixture is carried out in 1-3MPa hydrogen atmosphere under room temperature to stirring reaction, after 1-2h, stop stirring and take out solution, obtain the solution that contains Pt nano particle; The solution that contains Pt nano particle obtaining and metal oxide carrier are mixed, and magnetic agitation is adsorbed on metal oxide carrier Pt nano particle completely, filtering solution, the dry Pt/MO that obtains of washing xcatalyst.
Further, MO xfor TiO 2, SiO 2, ZrO 2, or Al 2o 3.
Further, Pt/MO xin catalyst, the load capacity of Pt is 0.1-1wt%, preferably 1%.
Further, magnetic agitation is spent the night, and Pt nano particle is adsorbed on metal oxide carrier completely.
Further, after filtering solution, filtrate recoverable.
Further, cleaning solvent is acetone.
In the present invention, Pt precursor Pt 2(dba) 3can prepare in accordance with the following steps: by appropriate dba(dibenzalacetone), sodium acetate and alcohol mixture pack in there-necked flask, stirring and dissolving at 50 ℃, adds appropriate K 2ptCl 4the aqueous solution, is heated at 90 ℃ and refluxes, and reacts 2 hours, stops heating, stirs and is cooled to room temperature, and hold over night, after filtration, with distilled water washing, then cleans with pentane, removes other reaction impurities.
The present invention also provides described Pt/MO xcatalyst is in the aflame application of toluene catalytically.
Concrete, described in be applied as: by prepared Pt/MO xcatalyst is placed in fixed-bed micro-reactor, and making toluene concentration is 1000-3000ppm, and the air speed of take is reacted as the condition of 18000-54000ml/ (g h).
The present invention utilizes X-ray diffractometer (XRD) to measure the crystal phase structure of catalyst, utilizes transmission electron microscope (TEM) to observe pattern and the pore structure of catalyst.Utilize gas-chromatography and flame ionic detector to measure the catalytic activity of catalyst to toluene oxidation.Result shows, adopts the synthetic Pt/MO of the method for the invention xthe performance with efficiently catalyzing and oxidizing toluene can realize toluene and be completely oxidized to carbon dioxide and water at the temperature lower than 110 ℃, and does not have other products to generate.
Pt/MO of the present invention xcatalyst for catalytic combustion is the catalyst that between a kind of active component and carrier, the mode by self assembly is combined into.It compared with prior art has following advantage: the synthetic method of catalyst of the present invention, and propylene glycol carbonate can reuse, and can not produce waste gas waste water, and Environmental costs are low, are easy to expansion scale and carry out industrial production; The catalyst activity making is high, good stability, can realize Low Concentration Toluene at low temperatures (lower than 110 ℃) be completely oxidized to carbon dioxide and water, and generate without other products.
Accompanying drawing explanation
Fig. 1 is Pt/MO at 110 ℃ xthe conversion ratio histogram of sample catalysis 1000ppm toluene.
Fig. 2 is Pt/Al 2o 3the conversion ratio of sample catalysis variable concentrations toluene and the graph of a relation of reaction temperature.
Fig. 3 is Pt/Al 2o 3the conversion ratio of the different GHSV toluene of sample catalysis and the graph of a relation of reaction temperature.
The specific embodiment
For further understanding the present invention, with embodiment, elaborate below, and provide accompanying drawing and describe the present invention and adopt Pt/MO xeffectively improve the performance of catalytic oxidation toluene.
Embodiment 1
Pt/MO xthe preparation of catalyst
By precursor 34mg Pt 2(dba) 3add 100ml propylene glycol carbonate, under 3.0MPa, room temperature (20 ℃), react 2 hours in stainless steel cauldron, obtaining reactant liquor is Pt nanoparticles solution 100ml; By carrier MO x(MO x=TiO 2, SiO 2, ZrO 2, Al 2o 3) join the Pt nanoparticles solution of acquisition, under electric power stirring action, stir and spend the night, filter, filter cake is dry after cleaning for several times with acetone, acquires 1%Pt/MO xcatalyst.
Embodiment 2
Take 0.5g Pt/TiO 2catalyst is placed in the quartz tube reactor that internal diameter is 8mm, and it is 1000ppm that adjustment gas flow makes the concentration of toluene, and reaction velocity (GHSV) is 18000ml/ (gh), and reaction temperature interval is from 80 ℃～180 ℃.Toluene concentration and product utilization gas Chromatographic Determination.
Reaction result shows, in the time of 110 ℃, after catalyst system, the conversion ratio of toluene reaches 98%.
Pt/TiO 2catalyst activity evaluation result is shown in accompanying drawing 1.
Embodiment 3
Take 0.5g Pt/SiO 2catalyst is placed in the quartz tube reactor that internal diameter is 8mm, and it is 1000ppm that adjustment gas flow makes the concentration of toluene, and reaction velocity (GHSV) is 18000ml/ (gh), and reaction temperature interval is from 80 ℃～180 ℃.Toluene concentration and product utilization gas Chromatographic Determination.
Reaction result shows, in the time of 110 ℃, after catalyst system, the conversion ratio of toluene reaches 100%.
Pt/SiO 2catalyst activity evaluation result is shown in accompanying drawing 1.
Embodiment 4
Take 0.5g Pt/ZrO 2catalyst is placed in the quartz tube reactor that internal diameter is 8mm, and it is 1000ppm that adjustment gas flow makes the concentration of toluene, and reaction velocity (GHSV) is 18000ml/ (gh), and reaction temperature interval is from 80 ℃～180 ℃.Toluene concentration and product utilization gas Chromatographic Determination.
Reaction result shows, in the time of 110 ℃, after catalyst system, the conversion ratio of toluene reaches 99%.
Pt/ZrO 2catalyst activity evaluation result is shown in accompanying drawing 1.
Embodiment 5
Take 0.5g Pt/Al 2o 3catalyst is placed in the quartz tube reactor that internal diameter is 8mm, and it is 1000ppm that adjustment gas flow makes the concentration of toluene, and reaction velocity (GHSV) is 18000ml/ (gh), and reaction temperature interval is from 80 ℃～180 ℃.Toluene concentration and product utilization gas Chromatographic Determination.
Reaction result shows, in the time of 110 ℃, after catalyst system, the conversion ratio of toluene reaches 100%.
Pt/Al 2o 3catalyst activity evaluation result is shown in attached Fig. 1 and 2.
Embodiment 6
Take 0.5g Pt/Al 2o 3catalyst is placed in the quartz tube reactor that internal diameter is 8mm, and it is 2000ppm that adjustment gas flow makes the concentration of toluene, and reaction velocity (GHSV) is 18000ml/ (gh), and reaction temperature interval is from 80 ℃～180 ℃.Toluene concentration and product utilization gas Chromatographic Determination.
Reaction result shows, in the time of 115 ℃, after catalyst system, the conversion ratio of toluene reaches 100%.
Pt/Al 2o 3catalyst activity evaluation result is shown in accompanying drawing 2.
Embodiment 7
Take 0.5g Pt/Al 2o 3catalyst is placed in the quartz tube reactor that internal diameter is 8mm, and it is 3000ppm that adjustment gas flow makes the concentration of toluene, and reaction velocity (GHSV) is 18000ml/ (gh), and reaction temperature interval is from 80 ℃～180 ℃.Toluene concentration and product utilization gas Chromatographic Determination.
Reaction result shows, in the time of 110 ℃, after catalyst system, the conversion ratio of toluene reaches 100%.
Pt/Al 2o 3catalyst activity evaluation result is shown in accompanying drawing 2.
Embodiment 8
Take 0.5g Pt/Al 2o 3catalyst is placed in the quartz tube reactor that internal diameter is 8mm, and it is 1000ppm that adjustment gas flow makes the concentration of toluene, and reaction velocity (GHSV) is 36000ml/ (gh), and reaction temperature interval is from 80 ℃～180 ℃.Toluene concentration and product utilization gas Chromatographic Determination.
Reaction result shows, in the time of 120 ℃, after catalyst system, the conversion ratio of toluene reaches 100%.
Pt/Al 2o 3catalyst activity evaluation result is shown in accompanying drawing 3.
Embodiment 9
Take 0.5g Pt/Al 2o 3catalyst is placed in the quartz tube reactor that internal diameter is 8mm, and it is 1000ppm that adjustment gas flow makes the concentration of toluene, and reaction velocity (GHSV) is 54000ml/ (gh), and reaction temperature interval is from 80 ℃～180 ℃.Toluene concentration and product utilization gas Chromatographic Determination.
Reaction result shows, in the time of 130 ℃, after catalyst system, the conversion ratio of toluene reaches 100%.
Pt/Al 2o 3catalyst activity evaluation result is shown in accompanying drawing 3.

Claims (5)

1. a Pt/MO xcatalyst, wherein MO xfor metal oxide, its preparation method comprises the steps: Pt 2(dba) 3join and in propylene glycol carbonate, obtain mixture, and this mixture is carried out in 1-3MPa hydrogen atmosphere under room temperature to stirring reaction, after 1-2h, stop stirring and take out solution, obtain the solution that contains Pt nano particle; The solution that contains Pt nano particle obtaining and metal oxide carrier are mixed, and magnetic agitation is adsorbed on metal oxide carrier Pt nano particle completely, filtering solution, the dry Pt/MO that obtains of washing xcatalyst.
2. Pt/MO as claimed in claim 1 xcatalyst, is characterized in that: MO xfor TiO 2, SiO 2, ZrO 2, or Al 2o 3.
3. Pt/MO as claimed in claim 1 or 2 xcatalyst, is characterized in that: Pt/MO xin catalyst, the load capacity of Pt is 0.1～1wt%.
4. Pt/MO as claimed in claim 1 xcatalyst, is characterized in that: after filtering solution, and filtrate recoverable.
5. Pt/MO as claimed in claim 1 xcatalyst, is characterized in that: cleaning solvent is acetone Pt/MO as claimed in claim 1 or 2 xcatalyst is in the aflame application of toluene catalytically.
CN201310459979.4A 2013-09-29 2013-09-29 Pt/MOx catalyst and application thereof in toluene catalytic combustion Pending CN103551141A (en)

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CN103599774A (en) * 2013-11-20 2014-02-26 浙江工业大学 Pt/Al2O3 catalyst and application thereof in room-temperature catalytic oxidation of formaldehyde
CN105536777A (en) * 2015-12-17 2016-05-04 杭州电子科技大学 Catalytic combustion active ingredient highly-dispersed catalyst and preparation method thereof
CN105817236A (en) * 2016-04-22 2016-08-03 宁波高新区夏远科技有限公司 Toluene low-temperature combustion catalyst and preparation method thereof
CN106362736A (en) * 2016-08-25 2017-02-01 浙江工业大学 Low-load palladium-platinum core-shell structure catalyst and preparation method and application thereof
CN106390998A (en) * 2016-08-30 2017-02-15 陈劲夫 Nanometer titania based composite catalyst and preparation method thereof
CN107159202A (en) * 2017-04-01 2017-09-15 浙江工业大学 A kind of supported palladium catalyst of additive Mn and preparation method and application
CN111097407A (en) * 2019-11-19 2020-05-05 浙江工业大学 Load type nano Pt/Al2O3Process for preparing catalyst
CN111151247A (en) * 2018-11-08 2020-05-15 中国科学院大连化学物理研究所 Supported catalyst and preparation method and application thereof
CN113198465A (en) * 2021-04-29 2021-08-03 浙江工业大学 Ruthenium-platinum alloy catalyst and application thereof
CN115518634A (en) * 2022-08-29 2022-12-27 江苏科技大学 Supported mesoporous silicon catalyst and preparation method and application thereof

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Cited By (14)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN103599774A (en) * 2013-11-20 2014-02-26 浙江工业大学 Pt/Al2O3 catalyst and application thereof in room-temperature catalytic oxidation of formaldehyde
CN105536777B (en) * 2015-12-17 2018-03-13 杭州电子科技大学 It is a kind of to be used to be catalyzed active component dispersed catalysts of burning and preparation method thereof
CN105536777A (en) * 2015-12-17 2016-05-04 杭州电子科技大学 Catalytic combustion active ingredient highly-dispersed catalyst and preparation method thereof
CN105817236A (en) * 2016-04-22 2016-08-03 宁波高新区夏远科技有限公司 Toluene low-temperature combustion catalyst and preparation method thereof
CN106362736A (en) * 2016-08-25 2017-02-01 浙江工业大学 Low-load palladium-platinum core-shell structure catalyst and preparation method and application thereof
CN106362736B (en) * 2016-08-25 2019-04-09 浙江工业大学 Low-load amount palladium platinum catalyst with core-casing structure and the preparation method and application thereof
CN106390998A (en) * 2016-08-30 2017-02-15 陈劲夫 Nanometer titania based composite catalyst and preparation method thereof
CN106390998B (en) * 2016-08-30 2019-06-21 惠州市登高达电业有限公司 A kind of nm TiO 2-base composite catalyst and preparation method thereof
CN107159202A (en) * 2017-04-01 2017-09-15 浙江工业大学 A kind of supported palladium catalyst of additive Mn and preparation method and application
CN107159202B (en) * 2017-04-01 2020-10-09 浙江工业大学 Manganese-doped palladium supported catalyst and preparation method and application thereof
CN111151247A (en) * 2018-11-08 2020-05-15 中国科学院大连化学物理研究所 Supported catalyst and preparation method and application thereof
CN111097407A (en) * 2019-11-19 2020-05-05 浙江工业大学 Load type nano Pt/Al2O3Process for preparing catalyst
CN113198465A (en) * 2021-04-29 2021-08-03 浙江工业大学 Ruthenium-platinum alloy catalyst and application thereof
CN115518634A (en) * 2022-08-29 2022-12-27 江苏科技大学 Supported mesoporous silicon catalyst and preparation method and application thereof

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Application publication date: 20140205