CN101245916A - Method for eliminating chloro-aromatics low temperature catalytic combustion - Google Patents
Method for eliminating chloro-aromatics low temperature catalytic combustion Download PDFInfo
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- CN101245916A CN101245916A CNA2008100350550A CN200810035055A CN101245916A CN 101245916 A CN101245916 A CN 101245916A CN A2008100350550 A CNA2008100350550 A CN A2008100350550A CN 200810035055 A CN200810035055 A CN 200810035055A CN 101245916 A CN101245916 A CN 101245916A
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- oxide
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- rare earth
- aromatic hydrocarbon
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Abstract
The invention discloses a method used for fully catalysing, burning and eliminating volatile pollutants such as aromatic hydrocarbon chloride in the environment. The invention takes a transition metal oxide and a rare earth oxide loaded by alumina, silica and zirconia as a catalyst which is then brought into a reactor by the air which is taken as oxidant; the chlorine-containing volatile aromatic hydrocarbon is completely combusted under the action of the catalyst and is then converted into carbon dioxide, hydrogen chloride and chlorine; the tail gas which has been completely burned can be absorbed by a diluted alkali solution (acid gases such as hydrogen chloride/chlorine, etc.) and are emptied then. The catalyst which is used by the method of the invention has high activity, generates no by-product, causes no secondary pollution, has strong chlorine poisoning resistance and long service life of catalyst, which is especially suitable for completely catalysing, burning and eliminating chlorine-containing organic compounds under low temperature, more particularly the pollutants of volatile chlorine-containing aromatic hydrocarbons.
Description
Technical field
The invention belongs to the catalytic combustion environmental protection technical field, specially refer to a kind of method that the easy-to-volatile chloroarene low-temperature catalytic burning is eliminated that is used for.
Background technology
The chlorine-containing volatile hydro carbons not only can cause serious harm to human beings'health, also can cause influence lasting, accumulation property to biosystem, and can destroy atmospheric ozone layer.It all is chloride organic compound that 12 persistent organic pollutions of classifying the first place as are arranged in the united nations environment project international treaties.The chlorine-containing volatile hydro carbons divides the aromatic hydrocarbon chloride, as chlorobenzene, dichloro-benzenes, and non-aromatic face cream fat hydro carbons chloride, as dichloroethanes, trichloro-ethylene, tetrachloro-ethylene, chloromethanes and methane polychloride etc., the former results from waft white, the heat treatment of chlorine-containing compound and the recovery of metal of the wood pulp of chloro oxidant; The latter mainly results from chlorine industry oxygen chlorine legal system and is equipped with industries such as vinyl chloride process, process hides, washing, pharmacy.Because the muriatic process of above-mentioned generation all relates to the industry of present stage national economy, the discharging of a large amount of chlorine-containing compounds is inevitable.Therefore, the pollution that is caused from source elimination chlorine-containing volatile hydro carbons does not also possess possibility at present.And the pollution that the method elimination chlorine-containing volatile hydro carbons of taking post processing is brought becomes unique feasible approaches and methods.
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 Koho JP 2001286729 A2, Jpn.Kokai Tokkyo Koho JP2001286730 A2, Jpn.Kokai Tokkyo Koho JP 2001286734 A2, Jpn.Kokai TokkyoKoho 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.Kokai?Tokkyo?Koho?JP?2002219364?A2
[2]Kiyono，Kenichi；Uchida，Masaaki；Adachi，Kentaro；Nishii，Kazuhiro，Jpn.Kokai?Tokkyo?Koho?JP?2001286729?A2
[3]Kiyono，Kenichi；Uchida，Masaaki；Adachi，Kentaro；Nishii，Kazuhiro，Jpn.Kokai?Tokkyo?Koho?JP?2001286730?A2
[4]Kajikawa，Osamu；Wang，Hsiang?Sheng；Kawase，Noboru；Maeda，Takeshi，Jpn.Kokai?Tokkyo?Koho?JP?2001009284?A2.
[5]Kiyono，Kenichi；Uchida，Masaaki；Adachi，Kentaro；Nishii，Kazuhiro，Jpn.Kokai?Tokkyo?Koho?JP?2001286734?A2
[6]Moriya，Yoshifumi；Nawama，Junichi；Tokumitsu，Shuzo，Jpn.Kokai?TokkyoKoho?JP?2001327869?A2
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 easy-to-volatile chloroarene low-temperature catalytic burning method that is used for, this method is a combustion catalyst with oxide carried rare earth oxide and transition metal oxide, its activity is high, no coupling product generates, do not cause secondary pollution, anti-fluorine poisoning ability is strong, catalyst life is long, be specially adapted to complete catalytic combustion and eliminate halogen-containing organic compound, especially effumability chloro-hydrocarbons pollutant.
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 oxide carrier load, wherein oxide carrier is commercially available aluminium oxide, zirconia, silica, and its content is 70～90wt%; Rare earth oxide is one or several composition of lanthana, cerium oxide, neodymia, oxidation Gadolinium, and its content is 1～10%; Transition metal oxide is one or several composition of cupric oxide, iron oxide, oxidation alum, manganese oxide, cobalt oxide, tungsten oxide, and its content is 9～25%.
Supported rare earth oxide and transition metal oxide adopt incipient impregnation method well known in the art on oxide.The presoma of rare earth oxide is selected from the nitrate of rare earth, the presoma of transition metal oxide is selected from nitrate, oxalates, acetate, carbonate.
The invention provides a kind of method that complete catalytic combustion is eliminated environment easy-to-volatile chloroarene pollutant that is used for, it is characterized in that, in the presence of catalyst, employing is brought reactor into as the air of oxidant, make the completing combustion under the effect of catalyst of chlorine-containing volatile aromatic hydrocarbon, chlorine-containing volatile aromatic hydrocarbon is transformed into carbon dioxide, hydrogen chloride and chlorine.Completing combustion tail gas 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 100～500 ℃, is preferably 150～450 ℃, especially 350 ℃;
Catalyst consumption, must be enough to make chlorine-containing volatile aromatic hydrocarbon existing under the situation at humid air, change into carbon dioxide and hydrogen chloride, generally speaking, the concentration of chlorine-containing volatile aromatic hydrocarbon is 0.05～5vol% in the waste gas of chlorine-containing volatile aromatic hydrocarbon, and every gram catalyst treatment exhausted air quantity is 10～40L per hour;
Said humid air is the air that contains steam, and its water concentration must satisfy the chlorine that reaction is generated and all be converted into hydrogen chloride, but can not make water become the mortifier of reaction, and the concentration of suitable water is 0.1～15vol% in the air.
Adopt method of the present invention, in humid air, under lower reaction temperature, in the presence of catalyst, can long-term and stably the chlorine-containing volatile aromatic hydrocarbon in the waste gas be transformed into carbon dioxide and hydrogen chloride, activity of such catalysts does not reduce.
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 chlorine-containing volatile arene pollutant in papermaking, pharmacy, process hides, washing and the chemical industry waste gas is eliminated.
The specific embodiment
Embodiment 1
With commercially available 25g cerous nitrate (Ce (NO
3)
3) 6H
2O and 60g copper nitrate Cu (NO
3)
2) 3H
2O is dissolved in the 80mL ionized water, and this solution places 50 ℃ constant temperature water bath to stir 0.5h; In this solution, add 70g γ-Al then
2O
3(surface area is 212m
2/ g), constantly stirring, liquid to be impregnated is by γ-Al
2O
3After all absorbing, static, aging 12h, 100 ℃ of dry 24h in baking oven move in the roaster then, temperature programming in air atmosphere, 1 ℃ of per minute is raised to 180 ℃, insulation 2h; Temperature programming again, 10 ℃ of per minutes are raised to 550 ℃ with temperature, during insulation 4h, can obtain 20%CuO-10%CeO
2/ γ-Al
2O
3(CuO: CeO by weight
2Be 2: 1) catalyst.
With implement 1 method make 22%Fe
2O
3-8%CeO
2/ γ-Al
2O
3(Fe by weight
2O
3: CeO
2Being 22: 8) catalyst is embodiment 2.
With implement 1 method make 25%MnO
2-2.5%CeO
2/ γ-Al
2O
3(MnO by weight
2: CeO
2Being 10: 1) catalyst is embodiment 3.
Embodiment 4
With commercially available 5.3g lanthanum nitrate (La (NO
3)
3) 6H
2O and copper nitrate 32g Cu (NO
3)
2) 3H
2O is dissolved in the 80mL ionized water, and this solution places 50 ℃ constant temperature water bath to stir 0.5h; In this solution, add 86g SiO then
2(surface area is 312m
2/ g), constantly stirring in the process, liquid to be impregnated is by SiO
2After all absorbing, static, aging 12h, 100 ℃ of dry 24h in baking oven move in the roaster then, roasting in air atmosphere, method can obtain 10%CuO-4%La shown in embodiment 1
2O
3/ SiO
2(CuO: La by weight
2O
3Be 5: 2) catalyst.
With implement 4 method make 20%NiO-4%La
2O
3/ SiO
2(NiO: La by weight
2O
3Being 5: 1) catalyst is embodiment 5.
With implement 4 method make 20%Co
2O
3-4%La
2O
3/ SiO
2(Co by weight
2O
3: La
2O
3Being 5: 1) catalyst is embodiment 6.
Embodiment 7
All catalyst chlorobenzene combustion activities are estimated in fixed bed little anti-(internal diameter 6mm quartz) and are carried out, 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, is that the humid air of 5vol% is mixed into reactor and burns with dry air, water concentration respectively then.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
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
Embodiment 8
The concentration of chloride aromatic hydrocarbon organic compound is controlled at 1～3%, be that the humid air of 0.5vol% is mixed into reactor and burns with dry air, water concentration respectively, the amount that every gram catalyst is per hour handled waste gas is 10L, at embodiment 3 catalyst 25%MnO
2-2.5%CeO
2/ γ-Al
2O
3Catalytic combustion properties to dissimilar chlorine-containing volatile arenes (CVOCs) is investigated, and the results are shown in Table 2.
The catalytic combustion result of the different chlorine-containing volatile chlorinated hydrocarbons of table 2
The result shows, 25%MnO
2-2.5%CeO
2/ γ Al
2O
3Catalyst all has good catalytic combustion properties to dissimilar chlorine-containing volatile arenes.
Embodiment 9
Change the concentration of chlorobenzene, water in air branch concentration is controlled at 0.45～5%, the amount that every gram catalyst is per hour handled waste gas is 20L, and reaction pressure is at 0.3～0.5Mpa, at 25%MnO
2-2.5%CeO
2/ γ-Al
2O
3, 20%NiO-4%La
2O
3/ SiO
2Investigated of the influence of variable concentrations chlorobenzene on the catalyst, the results are shown in Table 3 catalytic combustion properties.
Table 3 variable concentrations chlorobenzene is to 25%MnO
2-2.5%CeO
2/ γ-Al
2O
3, 20%NiO-4%La
2O
3/ SiO
2Catalyst is urged
Change the influence of combustibility
The result shows, 25%MnO
2-2.5%CeO
2/ γ-Al
2O
3, 20%NiO-4%La
2O
3/ SiO
2Catalyst has good catalytic combustion properties for the chlorobenzene of low concentration.Thus, the catalyst among the present invention can be widely used in the catalytic combustion elimination of variable concentrations (organic pollution that comprises low concentration and high concentration) chlorine-containing volatile arene.
Embodiment 10
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, air is a dry air, on embodiment 3 catalyst, investigated of the influence of different air speeds, the results are shown in Table 4 the chlorobenzene catalytic combustion properties.
Table 4 air speed is to 25%MnO
2-2.5%CeO
2/ γ-Al
2O
3The influence of catalyst combustibility
The result shows, 25%MnO
2-2.5%CeO
2/ γ-Al
2O
3Exhaust-gas treatment amount hourly can be up to 30L/g catalyst (pressing 90% chlorobenzene by conversion calculations) down at 375 ℃ on the catalyst, and this commercial Application for catalyst is very crucial and important beyond doubt.
Claims (4)
1. one kind is used for easy-to-volatile chloroarene low-temperature catalytic burning method, it is characterized in that, in the presence of catalyst, employing is brought reactor into as the air of oxidant, make the completing combustion under the effect of catalyst of chlorine-containing volatile aromatic hydrocarbon, chlorine-containing volatile aromatic hydrocarbon is transformed into carbon dioxide, hydrogen chloride and chlorine.Completing combustion tail gas 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 100～500 ℃, is preferably 150～450 ℃, especially 350 ℃;
Catalyst consumption, must be enough to make chlorine-containing volatile aromatic hydrocarbon existing under the situation at humid air, change into carbon dioxide and hydrogen chloride, generally speaking, the concentration of chlorine-containing volatile aromatic hydrocarbon is 0.05～5vol% in the waste gas of chlorine-containing volatile aromatic hydrocarbon, and every gram catalyst treatment exhausted air quantity is 10～30L per hour;
Said catalyst constitutes with oxide carried rare earth oxide and transition metal oxide, and wherein oxide is a kind of in commercially available aluminium oxide, silica, the zirconia, and its content is 70～90wt%; Rare earth oxide is one or several composition of lanthana, cerium oxide, neodymia, oxidation Gadolinium, and its content is 1～10wt%; Transition metal oxide is one or several composition of cupric oxide, iron oxide, oxidation alum, manganese oxide, cobalt oxide, tungsten oxide, and its content is 9～25wt%.
2. the described Preparation of catalysts method of claim 1, it is characterized in that: supported rare earth oxide and transition metal oxide adopt incipient impregnation method well known in the art on aluminium oxide, silica, zirconia, and the presoma that the presoma of rare earth oxide is selected from the nitrate of rare earth, transition metal oxide is selected from nitrate, oxalates, acetate, carbonate.
3. the described Preparation of catalysts method of claim 1 is characterized in that: the rare earth nitrades and the transition metal presoma of metering are mixed, are dissolved in a certain amount of deionized water, place 50 ℃ constant temperature water bath to stir 0.5h this solution; In this solution, add a certain amount of oxide carrier then, constantly stir, after liquid to be impregnated is all absorbed by described oxide carrier, static, aging 12h, 100 ℃ of dry 24h in baking oven then, move in the roaster temperature programming in air atmosphere, 1 ℃ of per minute, be raised to 180 ℃, insulation 2h; Temperature programming again, 10 ℃ of per minutes are raised to 550 ℃ with temperature, during insulation 4h, promptly get described support type rare earth oxide of claim 1 and catalyst of transition metal oxide.
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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Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101822997A (en) * | 2010-04-29 | 2010-09-08 | 杭州森发环保科技有限公司 | Preparation method of catalyst for purifying organic waste gas containing hydrochloric ether |
| CN102200287A (en) * | 2011-05-17 | 2011-09-28 | 华东理工大学 | Method for catalyzing and purifying low molecular oxygen-containing organic waste gases |
| CN105289584A (en) * | 2015-11-11 | 2016-02-03 | 福建紫荆环境工程技术有限公司 | Catalyst for catalytic combustion of chloralkane, preparation method and application thereof |
| CN106140175A (en) * | 2016-06-24 | 2016-11-23 | 江苏安琪尔废气净化有限公司 | A kind of be catalyzed burning fluorine-containing, the preparation method of chlorine VOCs catalyst |
| CN106890635A (en) * | 2017-03-22 | 2017-06-27 | 华东理工大学 | A kind of catalyst for chloride VOC low-temperature catalytic burning and its preparation method and application |
| CN107362820A (en) * | 2017-08-16 | 2017-11-21 | 杭州更蓝生物科技有限公司 | It is a kind of to be used to be catalyzed catalyst of chlorinated organics burning and preparation method thereof |
| CN108906044A (en) * | 2018-06-15 | 2018-11-30 | 中国科学院过程工程研究所 | A kind of manganese cerium ruthenium composite oxide catalysts and its preparation method and application |
| CN115254108A (en) * | 2022-07-12 | 2022-11-01 | 南京工业大学 | Preparation method and application of amorphous silica-alumina encapsulated metal oxide catalyst |
| CN115624973A (en) * | 2022-09-20 | 2023-01-20 | 中国船舶重工集团公司第七一八研究所 | Sulfur poisoning resistant monolithic catalyst and preparation method and application thereof |
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2008
- 2008-03-25 CN CNA2008100350550A patent/CN101245916A/en active Pending
Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101822997A (en) * | 2010-04-29 | 2010-09-08 | 杭州森发环保科技有限公司 | Preparation method of catalyst for purifying organic waste gas containing hydrochloric ether |
| CN102200287A (en) * | 2011-05-17 | 2011-09-28 | 华东理工大学 | Method for catalyzing and purifying low molecular oxygen-containing organic waste gases |
| CN105289584A (en) * | 2015-11-11 | 2016-02-03 | 福建紫荆环境工程技术有限公司 | Catalyst for catalytic combustion of chloralkane, preparation method and application thereof |
| CN106140175A (en) * | 2016-06-24 | 2016-11-23 | 江苏安琪尔废气净化有限公司 | A kind of be catalyzed burning fluorine-containing, the preparation method of chlorine VOCs catalyst |
| CN106890635A (en) * | 2017-03-22 | 2017-06-27 | 华东理工大学 | A kind of catalyst for chloride VOC low-temperature catalytic burning and its preparation method and application |
| CN107362820A (en) * | 2017-08-16 | 2017-11-21 | 杭州更蓝生物科技有限公司 | It is a kind of to be used to be catalyzed catalyst of chlorinated organics burning and preparation method thereof |
| CN108906044A (en) * | 2018-06-15 | 2018-11-30 | 中国科学院过程工程研究所 | A kind of manganese cerium ruthenium composite oxide catalysts and its preparation method and application |
| CN115254108A (en) * | 2022-07-12 | 2022-11-01 | 南京工业大学 | Preparation method and application of amorphous silica-alumina encapsulated metal oxide catalyst |
| CN115624973A (en) * | 2022-09-20 | 2023-01-20 | 中国船舶重工集团公司第七一八研究所 | Sulfur poisoning resistant monolithic catalyst and preparation method and application thereof |
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Open date: 20080820 |