CN102824909A - Catalyst for low-temperature catalytic combustion of volatile organic compounds and preparation method thereof - Google Patents
Catalyst for low-temperature catalytic combustion of volatile organic compounds and preparation method thereof Download PDFInfo
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- CN102824909A CN102824909A CN2012103026502A CN201210302650A CN102824909A CN 102824909 A CN102824909 A CN 102824909A CN 2012103026502 A CN2012103026502 A CN 2012103026502A CN 201210302650 A CN201210302650 A CN 201210302650A CN 102824909 A CN102824909 A CN 102824909A
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Abstract
The invention discloses a catalyst for low-temperature catalytic combustion of volatile organic compounds and a preparation method thereof, belonging to the technical fields of chemical catalyst and preparation technology thereof. The catalyst contains, by mass percent, 0.1 to 1 % of an active ingredient Pb, 74 to 99.4 % of a carrier Al2O3 and 0.5 to 25% of an auxiliary agent RE2O3, wherein a specific surface area of a composite oxide RE2O3- Al2O3 is 80 to 326 m<2>/g. The catalyst provided by the invention is simple in preparation technology, easy to produce in large scale, and has a very high catalytic activity for low-temperature complete oxidation reactions of benzene, toluene, xylene, ethyl acetate, ethanol and propane. Provided is a novel and high-efficiency catalyst which can be used for purification treatment of the volatile organic compounds in fields of industrial exhaust or indoor pollution.
Description
Technical field
The invention belongs to chemical catalyst and preparing technical field thereof, be specifically related to a kind of low-temperature catalytic combustion volatility organic matter Catalysts and its preparation method.
Background technology
Volatile organic matter (Volatile Organic Compounds is called for short VOCs) is meant that saturated vapor pressure is greater than 70Pa under the normal temperature, and boiling point is lower than 260 ℃ organic compound under the normal pressure.Mainly comprise aromatic hydrocarbon, aliphatic hydrocarbon, halogenated hydrocarbons, oxygen-containing hydrocarbon, terpene hydrocarbon, alcohol, aldehyde, ketone and ester etc.They are petrochemical industry, pharmacy, the major pollutants in the industry discharging waste gas such as print, spray paint.This type organic has toxicity mostly and with stench, part can also be carcinogenic, and most VOCs has destruction to ozone layer.Traditional organic waste-gas purification method has absorption method, condensation method and direct firing method etc., but their easy generation of secondary pollution, energy consumption are big, the restriction that is subject to organic exhaust gas concentration and temperature.And catalytic combustion technology is to be completely oxidized to carbon dioxide and water to VOCs, and it is low that this method has an initiation temperature, consuming little energy; Applied widely, almost can handle all VOCs; Can not generate pollutants such as NOx, non-secondary pollution; Equipment volume is little; Conversion ratio is high; It is low to start energy consumption, and can reclaim even advantage such as output heat energy, has become a kind of main method of purifying VOCs.Mostly the present catalyst that adopts of this method is loaded noble metal catalyst, like ((1) Catal Today, 1999 such as Pt, Pd, Ru, Au; 54:81 (2) Appl Catal B, 2012,111-112:218 (3) Chem Eng J; 2012,180:46) these loaded noble metal catalysts have low, the active high advantage of initiation temperature, but have shortcoming such as cost an arm and a leg, less stable, anti-poisoning capability are low simultaneously; Make its application receive certain restriction ((4) Chem Lett, 1999,8:801 (5) J Catal; 2005,232:96).Research shows that the adding of rare earth and oxide thereof can improve activity of such catalysts, improve the heat endurance of catalyst, the anti-sulphur that improves catalyst, anti-plumbous ability ((6) Appl Catal B; 2009; 88:305 (7) J Alloy Compd, 2004,374:387).
Summary of the invention
The object of the present invention is to provide a kind of low-temperature catalytic combustion volatility organic matter Catalysts and its preparation method; Catalyst preparation process of the present invention is simple; Be prone to amplify and produce; Benzene,toluene,xylene, ethyl acetate, ethanol, propane low temperature complete oxidation are had very high catalytic activity, are a kind of novel, catalyst efficiently, can be used for the volatile organic matter purified treatment of aspects such as industrial tail gas or indoor pollution.
For realizing above-mentioned purpose, the present invention adopts following technical scheme:
A kind of low-temperature catalytic combustion volatility organic matter catalyst contains active component Pd, carrier A l
2O
3And auxiliary agent RE
2O
3, the mass percent of each component is: active component Pd 0.1~1%, auxiliary agent RE
2O
30.5~25%, carrier A l
2O
374~99.4%.
Said auxiliary agent RE
2O
3Be Nd
2O
3, Eu
2O
3, Gd
2O
3, Yb
2O
3, Lu
2O
3In one or more mixture.Added the Al behind the rare-earth additive
2O
3The carrier specific area is 80~326m
2/ g.
The crystallite dimension of said active component Pd is 1~50nm.
A kind of method for preparing aforesaid low-temperature catalytic combustion volatility organic matter catalyst may further comprise the steps:
(1) method through co-precipitation prepares aluminium hydroxide and rare-earth hydroxide mixture;
(2) mixture 80~120 ℃ of dryings, 500~900 ℃ of roastings in air atmosphere of step (1) being obtained obtain RE
2O
3-Al
2O
3Composite oxides;
The precursor solution of the carrier incipient impregnation active component that (3) step (2) is obtained, 50~120 ℃ of dry down backs in 500~900 ℃ of roastings.
The presoma of active component described in the step (3) is the palladium metal inorganic salts-palladium nitrate of solubility.
Beneficial effect of the present invention: catalyst of the present invention has very high low-temperature catalytic activity to the catalyst combustion reaction of volatile organic matter such as benzene,toluene,xylene, hydro carbons, alcohol, aldehyde, ether, ester etc.; And preparation technology is simple; Compare with common loaded noble metal catalyst, its activity is more excellent.This type catalyst also is expected to be used for the catalytic combustion elimination of other volatile organic matter of air such as halogenated hydrocarbons, ketone etc.
Description of drawings
Fig. 1 is the TEM figure of catalyst among the embodiment 2.
Fig. 2 be embodiment 3 with Comparative Examples 1 in catalyst to benzene catalyst combustion reaction conversion rate curve.
The specific embodiment
To be described further through embodiment and Comparative Examples catalyst below, but embodiment of the present invention is not limited to following embodiment this invention.
Technical scheme of the present invention is following:
Low-temperature catalytic combustion volatility organic matter catalyst provided by the present invention, (1~50nm) is active component, with Al with the precious metal palladium nano particle
2O
3Be carrier, and rare earth RE
2O
3Be auxiliary agent, RE
2O
3-Al
2O
3The specific area of composite oxides is 80~326m
2/ g.Wherein the shared percentage by weight of palladium is 0.1~1% in the catalyst, RE
2O
3Accounting for percentage by weight is 0.5~25%, carrier A l
2O
3Accounting for percentage by weight is 74~99.4%.
Preparation of catalysts method of the present invention is characterized in that: the Al that has added rare-earth additive with the coprecipitation preparation
2O
3Carrier, RE
2O
3-Al
2O
3The composite oxides surface area is 80~326m
2/ g.With equi-volume impregnating load active component palladium, making palladium particle size is 1~50nm.Catalyst preparation step comprises successively:
(1) method through co-precipitation prepares aluminium hydroxide and rare-earth hydroxide mixture;
(2) with the above-mentioned hydroxide that obtains 80~120 ℃ of dryings, 500~900 ℃ of roastings in air atmosphere, obtain RE
2O
3-Al
2O
3Composite oxides;
(3) with the precursor solution of the above-mentioned composite oxides incipient impregnation active component that obtains, dry back is in 500~900 ℃ of roastings under 50~120 ℃ of substep conditions.
In above-mentioned Preparation of catalysts method, the palladium metal inorganic salts that the said active component presoma of step (3) is a solubility, preferred palladium nitrate.
Embodiment 1
Take by weighing the Al (NO of 56.2690g
3)
39H
2Nd (the NO of O and 3.2876g
3)
36H
2O places conical flask, adds water to 200ml, treat that salt dissolves fully after; Under electronic stirring condition, adding 28% ammoniacal liquor to solution PH is 8~10; After continue stirring 1h, sediment through leave standstill, centrifugal, 120 ℃ of baking 12h, back 800 ℃ of roasting 4h in the Muffle furnace air get composite oxides.The specific area that records composite oxides with physical adsorption appearance (Micromeritics ASAP 2020) is 186.8 m
2/ g.
Then, grinding is sieved, and gets 30~80 order composite oxide carriers, and employing equi-volume impregnating load quality mark is 0.5% Pd.Detailed process is: get certain volume Pd solution impregnating carrier, stir 5min, with ultrasonic echography 10 min, the back is 50 ℃ of baking 0.5h in baking oven; 80 ℃ of baking 0.5h, 100 ℃ of baking 12h change Muffle furnace subsequently over to; 800 ℃ of roasting 4h in air atmosphere, grinding is sieved, and gets catalyst.
In fixed bed reactors, estimate catalytic combustion properties, catalyst amount 0.1g, air speed is 22000h
-1, reaction gas is 500ppm C
6H
6, 20%O
2, all the other are N
2The programming rate of beds is 5 ℃/min in the course of reaction, adopts GC-9560 type gas chromatograph to carry out on-line analysis.The result shows that when reaction temperature was 200,250,300,350,400,450,500 ℃, the conversion ratio of benzene was respectively 3.85,89.67,99.92,100,100,100 and 100%.
Embodiment 2
RE
2O
3-Al
2O
3The preparation method of composite oxides and the mode of loading of precious metals pd are with embodiment 1, and different is that added rare earth nitrades is the Gd (NO of 0.5149g
3)
36H
2The sintering temperature of the oxide after the O, complex hydroxide and load P d is 600 ℃.
The specific area of using physical adsorption appearance to record composite oxides is 186.8 m
2/ g.Transmission electron microscope (like accompanying drawing 1) shows that the size of precious metal palladium particle in the catalyst is about 6nm.
The activity of such catalysts evaluation method is with embodiment 1.Experimental result shows that when reaction temperature was 200,250,300,350,400,450,500 ℃, the conversion ratio of benzene was respectively 10.85,64.89,99.65,99.97,100,100 and 100%.
Embodiment 3
RE
2O
3-Al
2O
3The preparation method of composite oxides and the mode of loading of precious metals pd are with embodiment 1, and different is that added rare earth nitrades is the Yb (NO of 0.7007g
3)
36H
2The sintering temperature of the oxide after the O, complex hydroxide and load P d is 600 ℃, and the load capacity of Pd is 0.1%.The specific area of using physical adsorption appearance to record composite oxides is 225.8 m
2/ g.
The activity of such catalysts evaluation method is with embodiment 1.The result shows that when reaction temperature was 200,247,300,348,401,450,503 ℃, the conversion ratio of benzene was respectively 0,10.63,98.09,100,100,100 and 100%.
Comparative Examples 1
Al
2O
3Mode of loading and the load capacity of preparation method and precious metals pd with embodiment 3, different is not add rare earth nitrades.Experiment gained Al
2O
3Specific area be 235.2 m
2/ g.
As a comparison, with the Pd/Al of top gained
2O
3Catalyst takes by weighing 0.1g, is 22000h in air speed
-1, benzene concentration is under the condition of 500ppm, the catalyst combustion reaction of testing its benzene is active.The result shows that when temperature was 203,255,305,356,406,452,500 ℃, the conversion ratio of benzene was respectively 0,19.09,67.02,98.15,99.38,99.96 and 99.97%.
Embodiment 4
RE
2O
3-Al
2O
3The preparation method of composite oxides and the mode of loading of precious metals pd are with embodiment 1, and different is that added rare earth nitrades is the Lu (NO of 0.3518g
3)
36H
2Yb (the NO of O and 0.3503g
3)
36H
2The sintering temperature of the oxide after the O, complex hydroxide and load P d is 700 ℃, and the load capacity of Pd is 0.1% in the catalyst.The specific area of gained composite oxides is 223.4 m
2/ g.
The activity of such catalysts evaluation method is with embodiment 1.The result shows that when temperature was 203,256,303,352,400,450,500 ℃, the conversion ratio of benzene was respectively 0,13.47,93.68,99.81,100,100 and 100%.
RE
2O
3-Al
2O
3The preparation method of composite oxides and the mode of loading of precious metals pd are with embodiment 1, and different is that added rare earth nitrades is the Lu (NO of 0.2345g
3)
36H
2Yb (the NO of O, 0.2336g
3)
36H
2O and 0.2257g Gd (NO
3)
36H
2The sintering temperature of the oxide after the mixture of O, complex hydroxide and load P d is 700 ℃, and the load capacity of Pd is 0.1% in the catalyst.The specific area of gained composite oxides is 247.2 m
2/ g.
The activity of such catalysts evaluation method is with embodiment 1.The result shows that when temperature was 201,247,299,350,400,450,500 ℃, the conversion ratio of benzene was respectively 0,10.63,98.69,100,100,100 and 100%.
The above is merely preferred embodiment of the present invention, and all equalizations of doing according to claim of the present invention change and modify, and all should belong to covering scope of the present invention.
Claims (7)
1. a low-temperature catalytic combustion volatility organic matter catalyst contains active component Pd, carrier A l
2O
3And auxiliary agent RE
2O
3, it is characterized in that: the mass percent of each component is in the said catalyst: active component Pd 0.1~1%, auxiliary agent RE
2O
30.5~25%, carrier A l
2O
374~99.4%.
2. low-temperature catalytic combustion volatility organic matter catalyst according to claim 1 is characterized in that: said auxiliary agent RE
2O
3Be Nd
2O
3, Eu
2O
3, Gd
2O
3, Yb
2O
3, Lu
2O
3In one or more mixture.
3. low-temperature catalytic combustion volatility organic matter catalyst according to claim 1 is characterized in that: added rare-earth additive RE
2O
3After Al
2O
3The carrier specific area is 80~326m
2/ g.
4. low-temperature catalytic combustion volatility organic matter catalyst according to claim 1 is characterized in that: the crystallite dimension of said active component Pd is 1~50nm.
5. method for preparing low-temperature catalytic combustion volatility organic matter catalyst as claimed in claim 1, it is characterized in that: described preparation method may further comprise the steps:
(1) method through co-precipitation prepares aluminium hydroxide and rare-earth hydroxide mixture;
(2) mixture 80~120 ℃ of dryings, 500~900 ℃ of roastings in air atmosphere of step (1) being obtained obtain RE
2O
3-Al
2O
3Composite oxides;
The precursor solution of the carrier incipient impregnation active component that (3) step (2) is obtained, 50~120 ℃ of dry down backs in 500~900 ℃ of roastings.
6. low-temperature catalytic combustion volatility organic matter Preparation of catalysts method according to claim 5 is characterized in that: the presoma of active component described in the step (3) is the palladium metal inorganic salts of solubility.
7. low-temperature catalytic combustion volatility organic matter Preparation of catalysts method according to claim 6 is characterized in that: the palladium metal inorganic salts of said solubility are palladium nitrate.
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Cited By (11)
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CN103386312A (en) * | 2013-08-04 | 2013-11-13 | 江苏安琪尔废气净化有限公司 | Method for preparing spherical shell type catalyst for catalytic combustion of VOCs (volatile organic compounds) |
CN103386304A (en) * | 2013-08-04 | 2013-11-13 | 江苏安琪尔废气净化有限公司 | Preparation method of catalyst for catalytic combustion of volatile organic compounds |
CN104874396A (en) * | 2015-04-03 | 2015-09-02 | 上海华峰新材料研发科技有限公司 | Catalytic combustion-based catalyst for removing low-concentration and volatile organic compounds and preparation method thereof |
CN106111157A (en) * | 2016-07-04 | 2016-11-16 | 上海纳米技术及应用国家工程研究中心有限公司 | A kind of catalyst for propane catalytic combustion elimination and preparation and application |
CN110124689A (en) * | 2019-05-31 | 2019-08-16 | 金华铂锐催化科技有限公司 | A kind of catalyst and preparation method thereof for the purification of kitchen garbage fermentation tail gas |
CN111054389A (en) * | 2019-11-25 | 2020-04-24 | 李俊鸿 | Methanol low-temperature heating catalyst and preparation method thereof |
CN112264007A (en) * | 2020-11-13 | 2021-01-26 | 中南大学 | Aromatic compound catalytic combustion catalyst and preparation and application thereof |
CN113181956A (en) * | 2021-05-10 | 2021-07-30 | 中国科学院大学 | Combined catalyst and method for treating nitrogen-containing volatile organic compound pollutants |
CN113908820A (en) * | 2021-09-30 | 2022-01-11 | 北京动力机械研究所 | Low-temperature combustion flame-stabilizing catalyst, combustor and application thereof |
CN113996291A (en) * | 2021-11-09 | 2022-02-01 | 康纳新型材料(杭州)有限公司 | Low-temperature HVOCs catalytic combustion catalyst, and preparation method and application thereof |
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CN103386304A (en) * | 2013-08-04 | 2013-11-13 | 江苏安琪尔废气净化有限公司 | Preparation method of catalyst for catalytic combustion of volatile organic compounds |
CN104874396A (en) * | 2015-04-03 | 2015-09-02 | 上海华峰新材料研发科技有限公司 | Catalytic combustion-based catalyst for removing low-concentration and volatile organic compounds and preparation method thereof |
CN106111157A (en) * | 2016-07-04 | 2016-11-16 | 上海纳米技术及应用国家工程研究中心有限公司 | A kind of catalyst for propane catalytic combustion elimination and preparation and application |
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CN111054389A (en) * | 2019-11-25 | 2020-04-24 | 李俊鸿 | Methanol low-temperature heating catalyst and preparation method thereof |
CN111054389B (en) * | 2019-11-25 | 2023-06-30 | 李俊鸿 | Methanol low-temperature heating catalyst and preparation method thereof |
CN112264007A (en) * | 2020-11-13 | 2021-01-26 | 中南大学 | Aromatic compound catalytic combustion catalyst and preparation and application thereof |
CN112264007B (en) * | 2020-11-13 | 2021-07-20 | 中南大学 | Aromatic compound catalytic combustion catalyst and preparation and application thereof |
CN113181956A (en) * | 2021-05-10 | 2021-07-30 | 中国科学院大学 | Combined catalyst and method for treating nitrogen-containing volatile organic compound pollutants |
WO2022194306A1 (en) * | 2021-05-10 | 2022-09-22 | 中国科学院大学 | Composite catalyst and method for treating nitrogen-containing volatile organic composite pollutants |
CN113908820A (en) * | 2021-09-30 | 2022-01-11 | 北京动力机械研究所 | Low-temperature combustion flame-stabilizing catalyst, combustor and application thereof |
CN113996291A (en) * | 2021-11-09 | 2022-02-01 | 康纳新型材料(杭州)有限公司 | Low-temperature HVOCs catalytic combustion catalyst, and preparation method and application thereof |
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