CN102698751A - Catalyst for eliminating chlorine-containing volatile organic compounds by low-temperature catalytic combustion - Google Patents
Catalyst for eliminating chlorine-containing volatile organic compounds by low-temperature catalytic combustion Download PDFInfo
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Abstract
The invention discloses a catalyst for eliminating chlorine-containing volatile organic compounds by low-temperature catalytic combustion. The catalyst mainly comprises a transition metal oxide-cerium oxide composite oxide carrier and ruthenium oxide loaded by the carrier, wherein a transition metal element is of Ti, Mn, Co, Fe, Cu and Ni. Air which is taken as an oxidant is brought into a reactor so as to transform the chlorine-containing volatile organic compounds to carbon dioxide, hydrogen chloride and chlorine, and full combustion tail gas can be absorbed by a dilute alkaline solution (hydrogen chloride/chlorine and other acidic gas) and then exhausted. The catalyst has the advantages of high catalytic activity, strong anti-chlorine poisoning capability and long service life of the catalyst, and is particularly suitable for eliminating the chlorine-containing organic compounds by low-temperature catalytic combustion.
Description
Technical field
The invention belongs to volatile organic compound catalytic combustion environmental protection technical field; Specially refer to a kind of ruthenium-oxide/transition metal oxide-cerium oxide catalyst that is used for chloride volatile organic compound low-temperature catalytic burning elimination and preparation method thereof, and a kind of method that complete catalytic combustion is eliminated the chloride volatile organic pollution of environment that is used for is provided.
Background technology
Chlorine-containing volatile organic compound not only can cause serious harm to human beings'health, also can cause lasting, cumulative influence 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; Like chlorobenzene, dichloro-benzenes; And non-fragrant fat hydrocarbon chloride; Like dichloroethanes, trichloro-ethylene, tetrachloro-ethylene, chloromethanes and methane polychloride etc., the former results from the bleaching of the wood pulp of chloro oxidant, the heat treatment of chlorine-containing compound and the recovery of metal; 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, also do not possess the possibility of pollution that elimination chlorine-containing volatile hydro carbons is caused from the source at present.And the pollution that the method elimination chlorine-containing volatile hydro carbons of taking post processing is brought becomes unique feasible approach and method.In addition, the burning of house refuse also will produce the dioxins materials of severe toxicity, and the generation of this type of material mainly comes from contained chlorobenzene in the rubbish, imperfect combustion and the polymerization at high temperature of chlorobenzene phenols presoma material.Therefore, generation how to control dioxins materials becomes the core of garbage incineration technology.
In recent years, the comprehensive regulation to volatile organic compound (VOCs) had received concern more and more widely.At present, for the removal of chlorinated organics, mainly contain two big types of technology of biodegradation and non-biodegradation.The normal methods such as direct burning, absorption method, absorption process, photocatalysis, catalytic hydrogenation and dechlorination, catalyzed aqueous vapour reformation, catalytic combustion that adopt of non-biodegradation.Flame combustion need carry out under higher temperature (1000 ℃), and energy consumption is big; And this method is disliked English (PCDD) and polychlorinated dibenzo (PCDF) also causing more highly toxic bioxin (Dioxins) pollutant aspect the chloride hydro carbons of processing like polychlorinated dibenzo-2.Absorption method is unsatisfactory for the treatment effect of low concentration pollutant, and its adsorption efficiency is extremely low.Methods such as biological processes, photocatalytic degradation, hydrogenation-dechlorination 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.
Production by Catalytic Combustion Process is to utilize catalyst that organic matter (250～400 ℃) below burning-point is closed with oxidation, generates nontoxic H
2O, CO
2Reach the less HCl of toxicity, thereby reach the purpose of purification.Catalytic combustion is obtaining using widely aspect the elimination volatile organic compound.In addition, a large amount of practices shows that through the mode of catalytic combustion the dioxin that produces in the burning process being carried out the quadric catalysis decomposition at low temperatures is one of most economical, feasible method, and wherein key is the exploitation of high activity, high stability catalyst.Because the hypertoxicity of this type of material, so the general presomas such as monochloro-benzene, dichloro-benzenes and chlorophenol that adopt carry out screening of catalyst and investigation as the model molecule under laboratory condition.
In general; In the catalytic combustion of chlorine-containing organic compounds; Noble metal catalyst exists that price is relatively costly, the active height of chlorination (being prone to the bigger many chlorine accessory substance of toxigenicity), be prone to generate the oxychlorination compound and poison, cause because of the loss of noble metal easily in the high-temperature region problem such as inactivation, makes the application of noble metal catalyst be restricted.Recent years, the catalyst of chlorine-containing organic compounds catalytic combustion mainly concentrates on transition metal oxide and the solid acid catalyst, but there is active not high shortcoming in this type of catalyst.The catalyst activity component of mainly using in the patent documentation has transition metal oxide to be UO
2, MnO
2, Co
3O
4, La
2O
3, CeO
2Deng and precious metals pt, Pd etc., carrier is SiO
2, Al
2O
3, TiO
2, ZrO
2Representational patent has JP 2002219364, JP 2001286729, JP 2001278630, JP 2001009284, JP2001286734, JP 2001327869, JP 10085559A2, U.S.Patent 4031149, U.S.Patent4059677, U.S.Patent 4065543, U.S.Patent 4561969, U.S.Patent 5811628, U.S.Patent 4169862, U.S.Patent 7052663 etc.
Summary of the invention
The objective of the invention is to disclose a kind of chloride volatile organic compound low-temperature catalytic burning method that is used for; This method is a combustion catalyst with the composite oxide supported ruthenium-oxide of transition metal oxide-cerium oxide; Its active height, anti-fluorine poisoning ability are strong; Catalyst life is long, is specially adapted to complete catalytic combustion and eliminates organic halogen compound, especially chloride volatile organic pollution.
The invention provides a kind of catalyst that chloride volatile organic compound low-temperature catalytic burning is eliminated that is used for; This catalyst mainly is made up of transition metal oxide, cerium oxide and ruthenium-oxide; Wherein transition metal oxide is one or several formation of titanium oxide, manganese oxide, cobalt oxide, iron oxide, cupric oxide, nickel oxide, and preferential transition metal oxide is a titanium oxide.The content of transition metal oxide is 1～15wt%, preferred 4～12wt%; Ruthenium-oxide content is 0.1～3wt%, preferred 1～1.5%; All the other are cerium oxide.
Transition metal oxide-cerium oxide composite oxides adopt the method for simple co-precipitation to make, and wherein the presoma of manganese oxide, cobalt oxide, iron oxide, cupric oxide, nickel oxide is selected from nitrate, oxalates, acetate, carbonate; The presoma of titanium oxide is selected from alkoxide, titanium tetrachloride, the titanium sulfate of titanium; The cerium oxide precursor body is selected from nitrate, ammonium salt.
The load of ruthenium-oxide can be adopted infusion process, coprecipitation, deposition-precipitation method etc., preferred infusion process, and the presoma of ruthenium-oxide is selected from ruthenic chloride.
The invention provides a kind of method that complete catalytic combustion is eliminated the chlorine-containing volatile organic pollution of environment that is used for; It is characterized in that; In the presence of catalyst; Employing is brought reactor into as the air of oxidant, is the completing combustion under the effect of catalyst of chloride volatile organic compound, and chlorine-containing volatile organic compound 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 0.1～0.5Mpa, especially 0.1Mpa, and near normal pressure, temperature is 100～400 ℃, is preferably 150～300 ℃, especially 250 ℃;
Catalyst consumption; Must be enough to make chloride volatile organic compound under there is situation in air; Change into carbon dioxide and hydrogen chloride; Generally speaking, the concentration of chloride VOC is 0.05～5vo1% in the waste gas of chloride volatile organic compound, and every gram catalyst treatment exhausted air quantity is 5～60L per hour.
Adopt method of the present invention, in air, under lower reaction temperature, in the presence of catalyst, can long-term and stably the chlorine-containing volatile organic compound 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, can be widely used in the catalytic combustion elimination of the chloride volatile organic pollution in papermaking, pharmacy, process hides, the washing and the low-temperature catalyzed purification of consumer waste incineration Zhong dioxins materials.
The specific embodiment
Embodiment 1
Commercially available 10g six nitric hydrate ceriums are dissolved in the 20ml deionized water, again the 0.21ml butyl titanate are added drop-wise in the above-mentioned solution, stir 30min as A solution; 7.5g NaOH and 50ml deionized water mix the back as B solution; The powerful stirring down is added to the B drips of solution in the A solution, stirring at room 2h, still aging 48h, and suction filtration, washing, drying move to roasting in the Muffle furnace more then.Its concrete roasting process is: 50 ℃ begin heating, carry out temperature programming with the heating rate of 2.5 ℃/min, keep 3h at 450 ℃, obtain titanium oxide-cerium oxide composite oxides, and titanium cerium atom ratio is 5: 95.After the taking-up catalyst is ground to guarantee that catalyst is Powdered.
Commercially available ruthenic chloride is mixed with the aqueous solution of 20g/L; With this solution impregnation of 2ml in the titanium oxide-cerium oxide composite oxide power of the above-mentioned preparation of 4g; Leave standstill 8h under the room temperature in the air, place 110 ℃ of baking ovens to carry out dry 12h, put into the Muffle furnace roasting again; Its roasting process is identical with above-mentioned composite oxides roasting process, obtains catalyst 1%Ru/Ti-CeO
2(5: 95)-1.With the fine catalyst compression molding, grind back screening 40～60 order particles after the taking-up.
Embodiment 2
Commercially available 10g six nitric hydrate ceriums are dissolved in the 20ml deionized water, and the titanium tetrachloride with 0.18ml is added drop-wise in the above-mentioned solution again, stirs 30min as A solution; 7.5g NaOH and 50ml deionized water mix the back as B solution; The powerful stirring down is added to the B drips of solution in the A solution stirring at room 2h, still aging 48h, suction filtration, washing, drying then; Move to roasting in the Muffle furnace again; Roasting process is identical with embodiment 1, obtains titanium oxide-cerium oxide composite oxides, and titanium cerium atom ratio is 5: 95.After the taking-up catalyst is ground to guarantee that catalyst is Powdered.Press the same method load ruthenium-oxide of embodiment 1, prepare catalyst 1%Ru/Ti-CeO
2(5: 95)-2.
Embodiment 3
Preparing titanium oxide content by embodiment 1 same method is 10% catalyst 1%Ru/Ti-CeO
2(1: 9).
Embodiment 4
Preparing titanium oxide content by embodiment 1 same method is 1% catalyst 1%Ru/Ti-CeO
2(1: 99).
Embodiment 5
Commercially available 10g six nitric hydrate ceriums are dissolved in the 20ml deionized water, and 50% manganese nitrate solution with 1.7ml is added drop-wise in the above-mentioned solution again, stirs 30min as A solution; 7.5g NaOH and 50ml deionized water mix the back as B solution; The powerful stirring down is added to the B drips of solution in the A solution stirring at room 2h, still aging 48h, suction filtration, washing, drying then; Move to roasting in the Muffle furnace again; Roasting process is identical with embodiment 1, obtains manganese oxide-cerium oxide composite oxides, and manganese cerium atom ratio is 5: 95.After the taking-up catalyst is ground to guarantee that catalyst is Powdered.Press the same method load ruthenium-oxide of embodiment 1, prepare catalyst 1%Ru/Mn-CeO
2(5: 95).
Embodiment 6
After commercially available 10g six nitric hydrate ceriums, 0.23g cabaltous nitrate hexahydrate and the mixing of 20ml deionized water, stir 30min as A solution; 7.5g NaOH and 50ml deionized water mix the back as B solution; The powerful stirring down is added to the B drips of solution in the A solution stirring at room 2h, still aging 48h, suction filtration, washing, drying then; Move to roasting in the Muffle furnace again; Roasting process is identical with embodiment 1, obtains cobalt oxide-cerium oxide composite oxides, and cobalt cerium atom ratio is 5: 95.After the taking-up catalyst is ground to guarantee that catalyst is Powdered, press embodiment 1, prepare catalyst 1%Ru/Co-CeO with quadrat method load ruthenium-oxide
2(5: 95).
Embodiment 7
All catalyst chlorobenzene combustion activities are estimated in fixed-bed micro-reactor (internal diameter 3mm is quartzy) 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 pump injections of U.S. Stoelting company to get into vaporizer, is mixed into reactor with air then and burns.Total flow adopts mass flowmenter control, and the concentration of chlorobenzene is controlled at 0.066vol%, and it is 12L that every gram catalyst is per hour handled exhausted air quantity, is 340m/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 are seen table 1, T in the table
10%, T
50%, T
90%Be respectively conversion ratio and reach 10%, 50%, 90% o'clock required reaction temperature.The key reaction product is carbon dioxide, hydrogen chloride and chlorine.
Chlorobenzene catalytic combustion properties on table 1 different catalysts
Embodiment 8
Embodiment 1 catalyst 1wt%Ru/Ti-CeO
2On-1 1; 2-dichloro-benzenes and m-Chlorophenol combustion activity are estimated in fixed-bed micro-reactor (internal diameter 3mm is quartzy) and are carried out; Catalyst consumption is 200mg, 1, and the concentration of 2-dichloro-benzenes and m-Chlorophenol is controlled at 0.066vol%; It is 12L that every gram catalyst is per hour handled exhausted air quantity, is 340m/h through the gas line speed of reactor.Reaction pressure is 0.1Mpa, 1, and the conversion ratio of 2-dichloro-benzenes and m-Chlorophenol and the relation of reaction temperature are seen table 2, T in the table
10%, T
50%, T
90%Be respectively conversion ratio and reach 10%, 50%, 90% o'clock required reaction temperature.The key reaction product is carbon dioxide, hydrogen chloride and chlorine.
Table 21,2-dichloro-benzenes and m-Chlorophenol are at 1wt%Ru/Ti-CeO
2Catalytic combustion properties on-1 catalyst
Embodiment 9
It is 12L that every gram catalyst is per hour handled exhausted air quantity, and reaction pressure is at 0.1Mpa, and maintain is at 250 ℃, and the concentration of chlorobenzene is 0.18vol%, uses air to be oxidizing gas, and air is a dry air, at embodiment 1 catalyst 1wt%Ru/Ti-CeO
2On-1, the conversion ratio of chlorobenzene maintains more than 95% in 75 hours, does not see catalysqt deactivation.
Claims (4)
1. one kind is used for the catalyst that chloride volatile organic compound low-temperature catalytic burning is eliminated; This catalyst mainly is made up of the ruthenium-oxide of transition metal oxide-cerium oxide composite oxides and load thereof; Wherein transition metal oxide is one or several formation of titanium oxide, manganese oxide, cobalt oxide, iron oxide, cupric oxide, nickel oxide, and preferential transition metal oxide is a titanium oxide; The content of transition metal oxide is 1～15wt%, preferred 4～12wt%; Ruthenium-oxide content is 0.1～3wt%, and is preferred 1～1.5%, and all the other are cerium oxide.
2. the said Preparation of catalysts method of claim 1; It is characterized in that: transition metal oxide-cerium oxide composite oxides adopt the method for simple co-precipitation to make, and wherein the presoma of manganese oxide, cobalt oxide is selected from nitrate, oxalates, acetate, carbonate; The presoma of titanium oxide is selected from alkoxide, the titanium tetrachloride of titanium; The cerium oxide precursor body is selected from nitrate, ammonium salt.
3. the said Preparation of catalysts method of claim 1, it is characterized in that: dipping method well known in the art is adopted in the load of ruthenium-oxide, and the presoma of ruthenium-oxide is selected from ruthenic chloride.
4. the low-temperature catalytic burning that is widely used in industrial waste gas, refuse, the chloride volatile organic compound of waste water according to the said catalyst that is used for chloride volatile organic compound low-temperature catalytic burning elimination of claim 1 is eliminated, especially the chloride volatile organic pollution in the industrial waste gas.
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| CN103185344A (en) * | 2012-12-13 | 2013-07-03 | 浙江海洋学院 | Process for processing organic waste gas by utilizing waste hydrogenation 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 |
| CN107442102A (en) * | 2017-08-16 | 2017-12-08 | 杭州更蓝生物科技有限公司 | A kind of catalyst for chlorinated organics catalysis burning and preparation method thereof |
| CN107597122A (en) * | 2017-11-09 | 2018-01-19 | 浙江宏晟技术转让服务有限公司 | A kind of handling process for chloride organic exhaust gas |
| CN107670658A (en) * | 2017-11-09 | 2018-02-09 | 上海纳米技术及应用国家工程研究中心有限公司 | Catalyst for chlorobenzene low-temperature catalytic burning and its preparation method and application |
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| CN103185344A (en) * | 2012-12-13 | 2013-07-03 | 浙江海洋学院 | Process for processing organic waste gas by utilizing waste hydrogenation catalyst |
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| 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 |
| CN107442102A (en) * | 2017-08-16 | 2017-12-08 | 杭州更蓝生物科技有限公司 | A kind of catalyst for chlorinated organics catalysis burning and preparation method thereof |
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| CN108283928A (en) * | 2018-01-12 | 2018-07-17 | 齐齐哈尔大学 | Nucleocapsid Co3O4-CeO2@Fe3O4 in-situ preparation methods |
| 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 |
| CN110064401A (en) * | 2019-06-06 | 2019-07-30 | 上海纳米技术及应用国家工程研究中心有限公司 | Preparation and product and application for the co-modified cobaltosic oxide catalyst of cerium nickel in vinyl chloride low-temperature catalytic burning |
| CN110813275A (en) * | 2019-11-08 | 2020-02-21 | 南京工业大学 | Titanium-based nano catalytic oxidation catalyst and preparation method and application thereof |
| CN110813275B (en) * | 2019-11-08 | 2021-01-05 | 南京工业大学 | Titanium-based nano catalytic oxidation catalyst and preparation method and application thereof |
| CN111203241A (en) * | 2020-02-16 | 2020-05-29 | 山东迅达化工集团有限公司 | Organic chlorine-containing waste gas treatment catalyst and preparation method thereof |
| CN111203241B (en) * | 2020-02-16 | 2022-05-27 | 山东迅达化工集团有限公司 | Organic chlorine-containing waste gas treatment catalyst and preparation method thereof |
| CN112108191A (en) * | 2020-09-13 | 2020-12-22 | 北京工业大学 | Ruthenium-cobalt-loaded alloy nano catalyst for low-temperature catalytic combustion of 1, 2-dichloroethane |
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| CN113198459A (en) * | 2021-03-29 | 2021-08-03 | 上海中船临港船舶装备有限公司 | Catalyst for low-temperature catalytic combustion and preparation method and application thereof |
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| 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 |
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Application publication date: 20121003 |