CN101347723A - Catalyst for eliminating chlorinated aromatic hydrocarbons by low-temperature catalytic combustion - Google Patents
Catalyst for eliminating chlorinated aromatic hydrocarbons by low-temperature catalytic combustion Download PDFInfo
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- CN101347723A CN101347723A CNA2008100425307A CN200810042530A CN101347723A CN 101347723 A CN101347723 A CN 101347723A CN A2008100425307 A CNA2008100425307 A CN A2008100425307A CN 200810042530 A CN200810042530 A CN 200810042530A CN 101347723 A CN101347723 A CN 101347723A
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Abstract
The invention discloses a catalyst used for the removal of volatile chlorination aromatic hydrocarbon by lower-temperature catalytic combustion; the catalyst is essentially composed of alumina carrier and rare earth oxide and transition metal oxide loaded on the alumina carrier; wherein, transition metal elements are Cu, Fe, V, Mn, Mo, Co and W, and the rare earth oxide is one or a plurality of lanthana, cerium oxide, neodymia and gadolinium oxide. The catalyst of the invention has high activity, no byproduct generated, no secondary pollution, strong capacity of chlorine poisoning resistance and long service life and is especially suitable for removing halogen-containing organic compounds by lower-temperature catalytic combustion, more particularly, volatile chlorine-containing aromatic hydrocarbon pollutants.
Description
Technical field
The invention belongs to the catalytic combustion environmental protection technical field; specially refer to a kind of transition metal-rare-earth composite oxide catalyst that is used for the elimination of easy-to-volatile chloroarene low-temperature catalytic burning and preparation method thereof, and a kind of method that complete catalytic combustion is eliminated environment easy-to-volatile chloroarene pollutant that is used for is provided.
Background technology
Problem of environmental pollution, especially growing air pollution is one of problem of paying close attention to most of 21st century people.(polychlorinated dibenzo-p-dioxins PCDD) exists persistent pollution to environment to ， dioxin-like compound except SOx, NOx, ozone, hydro carbons.The harm of dioxin-like compound is not only human beings'health, and biosystem is caused influence lasting, accumulation property, and destroys the ozone of atmosphere.The ， dioxin-like compound is listed in the organic pollution that the first persistent tool is poisoned in united nations environment project international treaties.One of dioxin-like compound source results from the poly of many chlorine arene compound, and more is the combination that results from solid carbon, oxygen, chlorine source.(Municipalsolid waste, MSW) in the burning process, in the presence of chlorine source and catalyst, the combustion process of organic compound all relates to the generation bioxin at MSW.A bioxin part is discharged into atmosphere with the form of waste gas, and a part is adhered to fume emission to atmosphere with the tiny solid particle.Key component-chlorine the source that produces bioxin mainly comes from the solid refuse of chlorine-containing compound, is equipped with the industrial refuse and the domestic waste that produce in the vinyl chloride process by the industrial refuse of the recovery technology of the heat treatment of the bleaching process of the wood pulp of chloro oxidant and chlorine-containing compound and metal, oxygen chlorine legal system in the large-scale chlorine industry and constitutes.Because above-mentioned generation and use chlorine-containing compound process all relate to the industry of present stage China's national economy, the discharging that produces the solid refuse of bioxin presoma in a large number is inevitable.
In recent years, the comprehensive regulation to volatile organic compound (VOCs) had received concern more and more widely.Methods such as flame combustion, catalytic combustion and absorption are to eliminate the common method of these pollutants.But flame combustion need carry out under higher temperature (1000 ℃), and energy consumption is big; And this method is also causing more highly toxic bioxin (Dioxins) pollutant aspect the chloride hydro carbons of processing, as many chlorodiphenyls and bioxin (PCDD) and polychlorinated dibenzo (PCDF).Absorption method as one of organic pollution common method is unsatisfactory for the treatment effect of low concentration pollutant, and its adsorption efficiency is extremely low.For the elimination of the chloride aromatic hydrocarbon of effumability, the method for multiple novelty has been proposed recently in succession, as biological processes, photocatalytic degradation, hydrogenation-dechlorination etc.But these methods are not to have defective technically, are exactly that disposal cost is high, all are in the laboratory research state mostly, are difficult for realizing industrialization, industrialization.
Advantages such as the pollution that catalytic combustion is eliminated organic compound is a kind of energy-conservation, economic, effective processing method, compares with flame combustion, and it has, and ignition temperature is low, the time of staying short, required reactor is little, secondary pollution is few.Therefore, catalytic combustion is obtaining using widely aspect the elimination volatile organic compound.
Chlorination aromatic hydrocarbon such as chlorobenzene, dichlorobenzene, dioxin, its catalytic combustion is mainly used in the exhaust-gas treatment of incinerator, and the research work of this direction and the exploitation of technology concentrate on Japan.Representational patent has Jpn.Kokai Tokkyo Kobo JP2001286729 A2, Jpn.Kokai Tokkyo Koho JP 2001286730 A2, Jpn.Kokai Tokkyo Koho JP2001286734 A2, Jpn.Kokai Tokkyo Koho JP 10085559 A2 etc.Use fuel gas and air to burn.The main catalyst activity component of using is transition metal and noble metal, and carrier is SiO
2, Al
2O
3, TiO
2, ZrO
2Though precious metal catalyst is active higher, is easy to fluorine poisoning; The anti-poisoning capability of non-precious metal catalyst is stronger, but selectivity is lower, often has polystream to produce.
Part chlorination aromatic hydrocarbon catalytic combustion granted patent has:
[1]Nawama，Junichi；Moriya，Yoshifumi；Suzuki，Tadashi；Kuchino，Kunikazu，Jpn.KokaiTokkyo Kobo JP 2002219364A2
[2]Kiyono，Kenichi；Uchida，Masaaki；Adachi，Kentaro；Nishii，Kazuhiro，Jpn.KokaiTokkyo Koho JP 2001286729A2
[3]Kiyono，Kenichi；Uchida，Masaaki；Adachi，Kentaro；Nishii，Kazuhiro，Jpn.KokaiTokkyo Kobo JP 2001286730A2
[4]Kajikawa，Osamu；Wang，Hsiang Sheng；Kawase，Noboru；Maeda，Takeshi，Jpn.KokaiTokkyo Koho JP 2001009284A2.
[5]Kiyono，Kenichi；Uchida，Masaaki；Adachi，Kentaro；Nishii，Kazuhiro，Jpn.KokaiTokkyo Koho JP 2001286734A2
[6]Moriya，Yoshifumi；Nawama，Junichi；Tokumitsu，Shuzo，Jpn.Kokai Tokkyo Koho JP2001327869A2
These patent works mainly are to be active component with the transition metal, and catalytic combustion purifies De bioxin in the incinerator.
All there is shortcoming more or less in the catalyst that above-mentioned chlorine-containing volatile hydro carbons catalytic combustion elimination is adopted, low as catalytic combustion activity, have the polychlorocarbon class to produce, easily cause secondary pollution in the catalyticing combustion process, the catalyst activity component runs off easily, catalyst life short.
Summary of the invention
The objective of the invention is to disclose a kind of transition metal-rare-earth composite oxide catalyst that is used for the elimination of easy-to-volatile chloroarene low-temperature catalytic burning and preparation method thereof.Such catalytic activity height, no coupling product generate, do not cause secondary pollution, anti-fluorine poisoning ability is strong, catalyst life is long, are specially adapted to catalytic combustion and eliminate halogen-containing organic compound, especially the chloride arene pollutant of effumability.
The invention provides a kind of catalyst that the easy-to-volatile chloroarene low-temperature catalytic burning is eliminated that is used for, this catalyst mainly is made of the rare earth oxide and the transition metal oxide of alumina support and load thereof, wherein oxidation of interim metal is one or several formation of cupric oxide, iron oxide, vanadium oxide, manganese oxide, molybdenum oxide, cobalt oxide, tungsten oxide, and preferred transition metal oxide is cupric oxide, iron oxide, manganese oxide; Rare earth oxide is one or several formation of lanthana, cerium oxide, neodymia, gadolinium oxide, and preferred rare earth oxide is lanthana, cerium oxide.The content of transition metal is 10～18wt% (oxide content), is preferably 14～18wt%; Rare earth oxide is 1～10%, is preferably 2～4wt.%; Alumina content is 80%.
The transition metal oxide of alumina support load and rare-earth composite oxide catalyst adopt sol-gal process to make, and the presoma of transition metal oxide is selected from nitrate, oxalates, acetate, carbonate; The rare earth oxide presoma is selected from the nitrate of rare earth, aluminium oxide presoma be selected from aluminum nitrate.
The invention provides a kind of method that catalytic combustion is eliminated environment effumability chlorine compound fragrant hydrocarbon that is used for.The invention provides following technology path:
In the presence of catalyst, adopt and bring reactor into as the air of oxidant, make the completing combustion under the effect of catalyst of the chloride compound fragrant hydrocarbon of effumability transform into carbon dioxide, hydrogen chloride and chlorine.Tail gas after catalytic combustion is handled can adopt dilute alkaline soln to absorb back emptying such as (hydrogen chloride/chlorine sour gas).
Reaction pressure is 0.1～1Mpa, preferred 0.1～0.5Mpa, especially 0.1Mpa, and near normal pressure, temperature is 150～450 ℃, is preferably 250～400 ℃, especially 400 ℃.
Catalyst consumption, must be enough to make chlorine-containing volatile aromatic hydrocarbon in the presence of air, change into carbon dioxide and hydrogen chloride, generally speaking, the concentration of the chloride compound fragrant hydrocarbon of effumability is 0.05～5vol% in the waste gas, and every gram catalyst treatment exhausted air quantity is 10～30L per hour.
Catalyst provided by the invention has characteristics such as preparation technology is simple, cheap, catalytic activity is high, anti-fluorine poisoning ability is strong, the life-span is long; Technology path is convenient and practical, and the catalytic combustion that can be widely used in the chloride arene pollutant of effumability in papermaking, pharmacy, process hides, washing and the chemical industry waste gas is eliminated.
The specific embodiment
Embodiment 1
With commercially available 4.1g cerous nitrate (Ce (NO
3)
36H
2O), 4.3g lanthanum nitrate (La (NO
3)
36H
2O), 680.4g aluminum nitrate (Al (NO
3)
36H
2O) be put into 40.9g manganese nitrate (Mn (NO
3)
2) in the 50wt% aqueous solution, add deionized water and make the volume of solution reach 350ml, the room temperature dissolving adds the 100g citric acid again, and makes its dissolving.This solution places 80 ℃ constant temperature water bath to stir 6～7h; Put into 110 ℃ the dry 12h of drying box then, move in the roaster, temperature programming in air atmosphere, 4.2 ℃ of per minutes are raised to 550 ℃, and insulation 5h can obtain 17.6%Mn
2O
3-1.2%CeO
2-1.2%La
2O
3-80%Al
2O
3Catalyst.Compressing tablet is pulverized 20-40 purpose particle, and is stand-by.
With implement 1 method make 16%Fe
2O
3-2%CeO
2-2%La
2O
3-80%Al
2O
3Catalyst is embodiment 2.
With implement 1 method make 16%Mn
2O
3-2%CeO
2-2%La
2O
3-80%Al
2O
3Catalyst is embodiment 3.
To implement 1 prepared 17.6%Mn
2O
3-1.2%CeO
2-1.2%La
2O
3-80%Al
2O
3Catalyst is embodiment 4 at 650 ℃ of roasting 5h.
To implement 1 prepared 17.6%Mn
2O
3-1.2%CeO
2-] .2%La
2O
3-80%Al
2O
3Catalyst is embodiment 5 at 750 ℃ of roasting 5h.
Embodiment 6
With commercially available 8.2g cerous nitrate (Ce (NO
3)
36H
2O), 680.4g aluminum nitrate (Al (NO
3)
36H
2O) be put into 40.9g manganese nitrate (Mn (NO
3)
2) in the 50wt% aqueous solution, add deionized water and make the volume of solution reach 350ml, the room temperature dissolving adds the 100g citric acid again, and makes its dissolving.This solution places 80 ℃ constant temperature water bath to stir 6～7h; Put into 110 ℃ the dry 12h of drying box then, move in the roaster, temperature programming in air atmosphere, 4.2 ℃ of per minutes are raised to 550 ℃, and insulation 5h can obtain 17.6%Mn
2O
3-2.4%CeO
2-80%Al
2O
3Catalyst.
Make 16%NiO-4%CeO with the method for implementing 6
2-80%Al
2O
3Catalyst is embodiment 7.
Make 16%Co with the method for implementing 6
2O
3-4%CeO
2-80%Al
2O
3Catalyst is embodiment 8.
Embodiment 9
The catalyst activity evaluation is carried out at fixed bed reactors.The chlorobenzene combustion activity test of all catalyst is all carried out in U-shaped quartzy little anti-(internal diameter 6mm), and catalyst consumption is 200mg, and temperature adopts K type thermocouple to control automatically.Chlorobenzene adopts 100 serial KDS120 type micro-injection pumps injections of U.S. Stoelting company to enter vaporizer, then with enter reactor after air mixes and burn.Total flow adopts mass flowmenter control, and the concentration of chlorobenzene is controlled at 0.1vol%, and the amount that every gram catalyst is per hour handled waste gas is 15L, is 120m/h through the gas line speed of reactor.Reaction pressure is 0.1Mpa, and the conversion ratio of chlorobenzene and the relation of reaction temperature see Table 1, T in the table 1
10%, T
50%, T
98%Be respectively conversion ratio and reach 10%, 50%, 98% o'clock required reaction temperature.The key reaction product is the chlorine of carbon dioxide, hydrogen chloride and trace.
Chlorobenzene catalytic combustion properties on table 1 different catalysts
| Catalyst | T 10％(℃) | T 50％(℃) | T 98％(℃) |
| Embodiment 1 | 103 | 185 | 260 |
| Embodiment 2 | 185 | 275 | 456 |
| Embodiment 3 | 112 | 189 | 263 |
| Embodiment 4 | 128 | 211 | 282 |
| Embodiment 5 | 253 | 311 | 415 |
| Embodiment 6 | 129 | 272 | 329 |
| Embodiment 7 | 136 | 271 | 532 |
| Embodiment 8 | 195 | 276 | 523 |
Embodiment 10
The concentration of polystream is controlled at 0.1～0.3%, and all the other are air, and the amount that every gram catalyst is per hour handled waste gas is 10L, have investigated the catalytic combustion properties of embodiment 1 catalyst to polystream, the results are shown in Table 2.
The catalytic combustion activity of polystream on table 2 embodiment 1 catalyst
| Chlorinated aromatic hydrocarbons | T 10％(℃) | T 50％(℃) | T 98％(℃) |
| Dichloro-benzenes | 122 | 236 | 292 |
| Trichlorine is stupid | 128 | 250 | 340 |
| Tetrachlorobenzene | 141 | 275 | 360 |
The result shows, 17.6%Mn
2O
3-2.4%CeO
2-80%Al
2O
3Catalyst all has good catalytic combustion properties to dissimilar polystream.
Embodiment 11
Change the concentration of chlorobenzene, water in air branch concentration is controlled at 0.45～1vol.%, the amount that every gram catalyst is per hour handled waste gas is 20L, and reaction pressure is at 0.3～0.5Mpa, at 17.6%Mn
2O
3-1.2%CeO
2-1.2%La
2O
3-80%Al
2O
3Investigate the catalytic combustion properties of variable concentrations chlorobenzene on the catalyst, the results are shown in Table 3.
Table 3 17.6%Mn
2O
3-1.2%CeO
2-1.2%La
2O
3-80%Al
2O
3Variable concentrations chlorobenzene catalytic combustion properties on the catalyst
The result shows, 17.6%Mn
2O
3-1.2%CeO
2-1.2%La
2O
3-80%Al
2O
3Catalyst has good catalytic combustion properties for the chlorobenzene of low concentration.This shows that catalyst of the present invention can be widely used in the catalytic combustion of variable concentrations (comprising low concentration and high concentration) the chloride compound fragrant hydrocarbon of effumability and eliminate.
Embodiment 12
Change every gram catalyst and per hour handle the amount of waste gas, reaction pressure is at 0.1Mpa, and the concentration of chlorobenzene is 0.1vol%, use air to be oxidizing gas, on embodiment 1 catalyst, investigated of the influence of different air speeds to the chlorobenzene catalytic combustion properties, the results are shown in Table 4.
Table 4 air speed 17.6%Mn
2O
3-1.2%CeO
2-1.2%La
2O
3-80%Al
2O
3The influence of catalyst combustibility
Embodiment 13
In the reaction unit of embodiment 9, the amount that every gram catalyst is per hour handled waste gas is 20L, is the chloride arene compound of effumability with the chlorobenzene, and reaction temperature is 400 ℃ and investigates 17.6%Mn
2O
3-1.2%CeO
2-1.2%La
2O
3-80%Al
2O
3The stability of catalyst activity in reaction atmosphere.After the result showed reaction 200h, the chlorobenzene conversion ratio did not detect polystream greater than 98% in the product.The commercial Application that this point is eliminated for the chlorine-containing volatile arene is particularly important, shows 17.6%Mn
2O
3-1.2%CeO
2-1.2%La
2O
3-80%Al
2O
3Catalyst has bigger application prospect aspect the exhaust fume catalytic processing of the chloride arene of industrial effumability.
Claims (4)
1. one kind is used for the catalyst that the easy-to-volatile chloroarene low-temperature catalytic burning is eliminated, this catalyst mainly is made of the rare earth oxide and the transition metal oxide of alumina support and load thereof, wherein transition metal oxide is one or several formation of cupric oxide, iron oxide, vanadium oxide, manganese oxide, molybdenum oxide, cobalt oxide, tungsten oxide, and preferred transition metal oxide is cupric oxide, iron oxide, manganese oxide; Rare earth oxide is one or several formation of lanthana, cerium oxide, neodymia, oxidation Gadolinium, and preferred rare earth oxide is lanthana, cerium oxide.The content of transition metal oxide is 10～18wt%, is preferably 14～18wt%; Rare earth oxide is 1～10%, is preferably 2～4wt.%; Alumina content is 80%.
2. the described Preparation of catalysts method of claim 1 is characterized in that: the transition metal oxide of alumina support load and rare earth oxide catalyst adopt the citric acid collosol and gel to make, and the rare earth oxide presoma is selected from the nitrate of rare earth; The presoma of transition metal oxide is selected from nitrate, oxalates, acetate, carbonate; The presoma of aluminium oxide is selected from aluminum nitrate.
3. the described Preparation of catalysts method of claim 2, it is characterized in that: rare earth nitrades, transition metal salt and the aluminum nitrate of metering are mixed, are dissolved in a certain amount of deionized water, add citric acid then, this solution places 80 ℃ constant temperature water bath to stir 6～7h; Put into 110 ℃ the dry 12h of drying box then, move in the roaster, temperature programming in air atmosphere, 4.2 ℃ of per minutes are raised to 550 ℃, are incubated 5h, promptly get the transition metal oxide and the rare earth oxide catalyst of the described alumina load of claim 2.
4. the low-temperature catalytic burning that is widely used in industrial waste gas, refuse, waste water easy-to-volatile chloroarene according to the described catalyst that is used for the elimination of easy-to-volatile chloroarene low-temperature catalytic burning of claim 1 is eliminated, especially the chloride arene pollutant of the effumability in the industrial waste gas.
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|---|---|---|---|
| CNA2008100425307A CN101347723A (en) | 2008-09-04 | 2008-09-04 | Catalyst for eliminating chlorinated aromatic hydrocarbons by low-temperature catalytic combustion |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNA2008100425307A CN101347723A (en) | 2008-09-04 | 2008-09-04 | Catalyst for eliminating chlorinated aromatic hydrocarbons by low-temperature catalytic combustion |
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|---|---|
| CN101347723A true CN101347723A (en) | 2009-01-21 |
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|---|---|---|---|
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102353065A (en) * | 2011-06-28 | 2012-02-15 | 华东理工大学 | Method for eliminating chlorinated aliphatic hydrocarbons through low temperature catalytic combustion |
| CN102784557A (en) * | 2011-05-18 | 2012-11-21 | 王文初 | Method and device for treating pharmaceutical and chemical waste gases |
| CN107149942A (en) * | 2016-11-30 | 2017-09-12 | 江苏安琪尔废气净化有限公司 | For the preparation method for the catalyst for being catalyzed burning polycyclic aromatic hydrocarbons (PAH) |
| CN109261144A (en) * | 2017-11-09 | 2019-01-25 | 新昌县以琳环保科技有限公司 | Catalyst for the technique of VOCs treatment containing chlorine |
| CN109967085A (en) * | 2019-03-18 | 2019-07-05 | 华南理工大学 | A kind of fento composite molecular screen film catalyst and the preparation method and application thereof of catalysis burning volatile organic compounds containing chlorine |
| CN111921532A (en) * | 2020-09-07 | 2020-11-13 | 山东大学 | VOCs waste gas catalytic oxidation catalyst, preparation method thereof, catalytic oxidation device and method |
| CN113649022A (en) * | 2021-10-20 | 2021-11-16 | 天津环科环境咨询有限公司 | Catalyst for catalytic combustion of organic volatile waste gas and preparation method thereof |
| CN113944937A (en) * | 2021-11-15 | 2022-01-18 | 浙江传化合成材料有限公司 | Efficient treatment and comprehensive utilization method for butadiene rubber waste gas |
-
2008
- 2008-09-04 CN CNA2008100425307A patent/CN101347723A/en active Pending
Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102784557A (en) * | 2011-05-18 | 2012-11-21 | 王文初 | Method and device for treating pharmaceutical and chemical waste gases |
| CN102353065A (en) * | 2011-06-28 | 2012-02-15 | 华东理工大学 | Method for eliminating chlorinated aliphatic hydrocarbons through low temperature catalytic combustion |
| CN107149942A (en) * | 2016-11-30 | 2017-09-12 | 江苏安琪尔废气净化有限公司 | For the preparation method for the catalyst for being catalyzed burning polycyclic aromatic hydrocarbons (PAH) |
| CN109261144A (en) * | 2017-11-09 | 2019-01-25 | 新昌县以琳环保科技有限公司 | Catalyst for the technique of VOCs treatment containing chlorine |
| CN109261144B (en) * | 2017-11-09 | 2021-08-31 | 烟台百川汇通科技有限公司 | Catalyst for chlorine-containing organic waste gas treatment process |
| CN109967085A (en) * | 2019-03-18 | 2019-07-05 | 华南理工大学 | A kind of fento composite molecular screen film catalyst and the preparation method and application thereof of catalysis burning volatile organic compounds containing chlorine |
| CN111921532A (en) * | 2020-09-07 | 2020-11-13 | 山东大学 | VOCs waste gas catalytic oxidation catalyst, preparation method thereof, catalytic oxidation device and method |
| CN113649022A (en) * | 2021-10-20 | 2021-11-16 | 天津环科环境咨询有限公司 | Catalyst for catalytic combustion of organic volatile waste gas and preparation method thereof |
| CN113944937A (en) * | 2021-11-15 | 2022-01-18 | 浙江传化合成材料有限公司 | Efficient treatment and comprehensive utilization method for butadiene rubber waste gas |
| CN113944937B (en) * | 2021-11-15 | 2022-08-09 | 浙江传化合成材料有限公司 | Efficient treatment and comprehensive utilization method for butadiene rubber waste gas |
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Open date: 20090121 |