CN108607544A - A kind of volatile organic matter low-temperature catalytic oxidation catalyst and its preparation and application - Google Patents
A kind of volatile organic matter low-temperature catalytic oxidation catalyst and its preparation and application Download PDFInfo
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- CN108607544A CN108607544A CN201810414306.XA CN201810414306A CN108607544A CN 108607544 A CN108607544 A CN 108607544A CN 201810414306 A CN201810414306 A CN 201810414306A CN 108607544 A CN108607544 A CN 108607544A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/002—Mixed oxides other than spinels, e.g. perovskite
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/32—Manganese, technetium or rhenium
- B01J23/34—Manganese
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/40—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the pentasil type, e.g. types ZSM-5, ZSM-8 or ZSM-11, as exemplified by patent documents US3702886, GB1334243 and US3709979, respectively
- B01J29/48—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the pentasil type, e.g. types ZSM-5, ZSM-8 or ZSM-11, as exemplified by patent documents US3702886, GB1334243 and US3709979, respectively containing arsenic, antimony, bismuth, vanadium, niobium tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
- B01D2257/702—Hydrocarbons
- B01D2257/7027—Aromatic hydrocarbons
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2523/00—Constitutive chemical elements of heterogeneous catalysts
Abstract
The invention belongs to chemical catalyst and its preparing technical field, specifically a kind of volatile organic matter low-temperature catalytic oxidation catalyst and its preparation and application.Catalyst activity component is manganese, zirconium and tin;Its molar ratio is followed successively by (0.60 0.90):(0.05‑0.20):(0.05‑0.20).The VOCs low-temperature oxidation catalyst preparation processes of the present invention are simple, there is very high catalytic activity and stability to the low-temperature catalytic oxidation reaction of the Typical Volatile Organics such as toluene, 100% can reach to the catalysis oxidation efficiency of Low Concentration Toluene in 300 DEG C or less all catalyst, be a kind of New high-efficient low-cost catalyst for being suitable for benzene series hydrocarbon low-temperature catalytic oxidation and eliminating.
Description
Technical field
The invention belongs to chemical catalyst and its preparing technical field, specifically a kind of volatile organic matter low temperature is urged
Change oxidation catalyst and its preparation and application.
Background technology
Volatile organic matter (Volatile Organic Compounds, abbreviation VOCs) refers to one kind in 20 DEG C of conditions
Lower vapour pressure is greater than or equal to 0.01kPa, and boiling point is in 250 DEG C of organic compounds below under normal pressure.It, can be with according to chemical constitution
It is further divided into:Alkanes, aromatic hydrocarbons, olefines, esters, halogenated hydrocarbon, aldehydes, ketone and other etc. eight classes.The source of VOCs
Extensively, it can be divided mainly into two class of outdoor source and indoor source.Outdoor source includes the exhaust gas that petrochemical industry is discharged;Papermaking,
The organic solvent that the industries such as paint, pesticide, rubber and weaving are discharged;The modern means of communication such as automobile, aircraft, steamer institute
The tail gas of discharge.Indoor source mostlys come from ornament materials and detergent.One of main source as atmosphere pollution,
The discharge of VOCs all constitutes serious harm for atmospheric environment and human health.On the one hand, volatile organic waste gas at
Divide complexity various, with SOx、NOxSeries of chemical occurs under certain condition Deng other gas pollutants and particulate matter etc.,
Then secondary pollution is generated, causes Organic aerosol to generate, air organic acid concentration increases and the environment such as photochemical fog
Problem;On the other hand, the VOCs being discharged into air has toxicity and carcinogenesis mostly, and with the irritations gas such as stench
Taste seriously affects health and the daily life of people.Traditional purification of volatile organic waste gas method has absorption method, condensation
Method and direct burning method, process costs are high, purification efficiency is low and is also easy to produce secondary pollution,
VOCs can be effectively removed using low-temperature catalytic oxidation technology at a lower temperature, be translated into carbon dioxide and
Water has a vast market application prospect.The core of the technology is the exploitation of high performance catalyst, currently used for the technology
Catalyst is broadly divided into carried noble metal, transition metal oxide and acidic molecular sieve etc..Loaded noble metal catalyst
With highest catalytic activity, but it is easy to inactivate because of high temperature sintering and poisoning in its with high costs and reaction;Metal oxide
Catalyst (such as Ce, Mn, Co oxide or composite oxides) has higher oxidation activity, anti-poisoning capability and lower life
Cost is produced, however its specific surface area is small, pore structure is single etc. limits the further promotion of its catalytic activity;Molecular sieve has height
Specific surface area, regular duct and surface acidity can be used for the catalysis oxidation of the VOCs containing chlorine directly as catalyst, while also may be used
It is used for the catalysis oxidation of a variety of VOCs as the carrier material of a variety of loaded catalysts, however is also easy to produce on single molecular sieve
The problem of organic by-products and carbon distribution, still needs to solve.
Invention content
Present invention aims at a kind of VOCs low-temperature catalytic oxidations catalyst of offer and its preparations and application.
To achieve the above object, the invention adopts a technical scheme as:
A kind of volatile organic matter (VOCs) low-temperature catalytic oxidation catalyst, catalyst activity component are manganese, zirconium and tin;Its
Molar ratio is followed successively by (0.60-0.90):(0.05-0.20):(0.05-0.20).
The catalyst is that the metal salt solution containing manganese, zirconium and tin is mixed with citric acid solution, after drying, roasting i.e.
For VOCs low-temperature oxidation catalysts;Wherein, the molar ratio of citric acid and metal salt is 0.8-1.4.
It is preferred that each metal component molar ratio is Zr/ (Mn+Zr+Sn)=0.1, Sn/ (Mn+Zr+Sn)=0.1.
A kind of volatile organic matter (VOCs) low-temperature catalytic oxidation catalyst, catalyst are the metal containing manganese, zirconium and tin
Salt is carried on carrier, wherein active component is that manganese, zirconium and tin molar ratio are followed successively by (0.60-0.90):(0.05-0.20):
(0.05-0.20);For catalyst activity component load capacity in terms of Mn elements, load capacity is 0.01-0.03mol Mn/10g carriers, excellent
It is 0.02molMn/10g carriers to select load capacity.
The catalyst be to contain the metal salt of manganese, zirconium and tin as maceration extract, by carrier impregnation in wherein, and after pass through
It is the VOCs low-temperature oxidation catalysts of support type after drying, roasting.
It is described containing manganese Metal salt be manganese nitrate, containing zirconium metal salt be zirconium nitrate, containing tin metal salt be stannic chloride.
A kind of preparation method of volatile organic matter low-temperature catalytic oxidation catalyst:
1) manganese Metal salt, zirconium metal salt and tin metal salt are mixed according to aforementioned proportion with citric acid solution, is then stirred
For use after mixing, citric acid is 0.8-1.4 with metal salt molar ratio;
2) above-mentioned mixed solution under 60-80 DEG C of oil bath is stirred into 6-8h, is positioned over 100-120 DEG C of oven drying 12-
20h, 400-600 DEG C of roasting 4-6h are gained catalyst after roasting.
Or, will contain manganese Metal salt, zirconium metal salt and tin metal mixed salt solution as maceration extract according to aforementioned proportion, to
Carrier is added in maceration extract, 100-120 DEG C of oven drying 12-20h, 400-600 DEG C of roasting 4-6h is positioned over after stirring, after roasting i.e.
For gained catalyst;For catalyst activity component load capacity in terms of Mn elements, load capacity is 0.01-0.03mol Mn/10g carriers.
The roasting roasts 4-6h with the heating rate of 5-8 DEG C/min at 400-600 DEG C, is granulated, grinds after roasting, sieve
Divide to 60-80 mesh to get catalyst;Preferred calcination temperature is 500 DEG C, time 4h.
The carrier is γ types aluminium oxide or H-type ZSM-5 molecular sieve;Preferred vector is H-type ZSM-5 molecular sieve.
A kind of application of volatile organic matter low-temperature catalytic oxidation catalyst, the catalyst have as light-concentration volatile
The catalysis material of machine catalytic purification of exhaust gases.It is preferred that the catalysis material of Low Concentration Toluene low-temperature catalytic oxidation.
Advantage for present invention:
Catalyst of the present invention does not add any noble metal component, using multicomponent composite catalyst, significantly improves catalyst
Activity;The gama-alumina or H-type ZSM-5 molecular sieve carrier for adding high-specific surface area, can significantly improve the absorption of catalyst
Performance, reaction contact time is long, and then improves catalytic efficiency;Catalyst is recyclable to be used for multiple times, and higher catalysis is maintained to live
Property;The present invention makes volatile organic matter in industrial waste gas and air react using catalyst, the typical cases such as 300 DEG C of Toluenes
VOCs conversion ratios can reach 100%, and then realize the qualified discharge of exhaust gas.
Simultaneously compared with prior art, excellent results of the invention are:
(1) compared to loaded noble metal catalyst, catalyst preparation of the invention is of low cost, has to VOCs higher
Catalytic purification efficiency;
(2) catalyst activity prepared by the method for the present invention is high, low for the complete conversion temperature of 1000ppm toluene
In 300 DEG C.
Description of the drawings
Fig. 1 is catalytic activity figure of the 2,4,6 gained catalyst of the embodiment of the present invention in toluene catalytic oxidation reaction.
Fig. 2 is catalytic activity figure of the 7,9 gained catalyst of the embodiment of the present invention in toluene catalytic oxidation reaction.
Specific implementation mode
With reference to embodiment, the present invention will be further described, but not limited to this.
Embodiment 1
3.22g manganese nitrate solutions (mass fraction 50%) and 6.4g citric acid solutions are mixed into (mass fraction 30%),
2.15g zirconium nitrates and 0.13g stannic chlorides are added again under stirring condition, are stirred as solution;By above-mentioned mixed solution 80
6h is stirred under DEG C oil bath, is positioned over 120 DEG C of oven drying 12h, 400 DEG C of roasting 4h (heating rates:5 DEG C/min), it is passed through after roasting
It is granulated, grinds, being sized to 60-80 mesh to get MnZrSn catalyst.
Embodiment 2
3.22g manganese nitrate solutions (mass fraction 50%) and 6.4g citric acid solutions are mixed into (mass fraction 30%),
2.15g zirconium nitrates and 0.13g stannic chlorides are added again under stirring condition, are stirred as solution;By above-mentioned mixed solution 80
6h is stirred under DEG C oil bath, is positioned over 120 DEG C of oven drying 12h, 500 DEG C of roasting 4h (heating rates:5 DEG C/min), it is passed through after roasting
It is granulated, grinds, being sized to 60-80 mesh to get MnZrSn catalyst.
Embodiment 3
3.22g manganese nitrate solutions (mass fraction 50%) and 6.4g citric acid solutions are mixed into (mass fraction 30%),
2.15g zirconium nitrates and 0.13g stannic chlorides are added again under stirring condition, are stirred as solution;By above-mentioned mixed solution 80
6h is stirred under DEG C oil bath, is positioned over 120 DEG C of oven drying 12h, 600 DEG C of roasting 4h (heating rates:5 DEG C/min), it is passed through after roasting
It is granulated, grinds, being sized to 60-80 mesh to get MnZrSn catalyst.
Embodiment 4
2.86g manganese nitrate solutions (mass fraction 50%) and 6.4g citric acid solutions are mixed into (mass fraction 30%),
4.30g zirconium nitrates and 0.26g stannic chlorides are added again under stirring condition, are stirred as solution;By above-mentioned mixed solution 80
6h is stirred under DEG C oil bath, is positioned over 120 DEG C of oven drying 12h, 500 DEG C of roasting 4h (heating rates:5 DEG C/min), it is passed through after roasting
It is granulated, grinds, being sized to 60-80 mesh to get MnZrSn catalyst.
Embodiment 5
2.51g manganese nitrate solutions (mass fraction 50%) and 6.4g citric acid solutions are mixed into (mass fraction 30%),
6.45g zirconium nitrates and 0.13g stannic chlorides are added again under stirring condition, are stirred as solution;By above-mentioned mixed solution 80
6h is stirred under DEG C oil bath, is positioned over 120 DEG C of oven drying 12h, 400 DEG C of roasting 4h (heating rates:5 DEG C/min), it is passed through after roasting
It is granulated, grinds, being sized to 60-80 mesh to get MnZrSn catalyst.
Embodiment 6
2.15g manganese nitrate solutions (mass fraction 50%) and 6.4g citric acid solutions are mixed into (mass fraction 30%),
8.59g zirconium nitrates and 0.52g stannic chlorides are added again under stirring condition, are stirred as solution;By above-mentioned mixed solution 80
6h is stirred under DEG C oil bath, is positioned over 120 DEG C of oven drying 12h, 500 DEG C of roasting 4h (heating rates:5 DEG C/min), it is passed through after roasting
It is granulated, grinds, being sized to 60-80 mesh to get MnZrSn catalyst.
Embodiment 7
4.30g zirconium nitrates and 0.26g stannic chlorides are added in 2.86g manganese nitrate solutions (mass fraction 50%), stirred
It mixes to be uniformly mixed and is used as maceration extract, 5g γ type aluminium oxide is added into maceration extract, 120 DEG C of oven drying 12h are positioned over after stirring,
4h (heating rates are roasted at 500 DEG C:5 DEG C/min), after roasting through granulation, grind, be sized to 60-80 mesh to get support type
MnZrSn/Al2O3Catalyst.
Embodiment 8
4.30g zirconium nitrates and 0.26g stannic chlorides are added in 2.86g manganese nitrate solutions (mass fraction 50%), stirred
It mixes to be uniformly mixed and is used as maceration extract, 10g H-type ZSM-5 molecular sieves are added to maceration extract, 120 DEG C of oven dryings are positioned over after stirring
12h roasts 4h (heating rates at 500 DEG C:5 DEG C/min), after roasting through granulation, grind, be sized to 60-80 mesh to get negative
The MnZrSn/HZSM-5 catalyst of load type.
Embodiment 9
4.30g zirconium nitrates and 0.26g stannic chlorides are added in 2.86g manganese nitrate solutions (mass fraction 50%), stirred
It mixes to be uniformly mixed and is used as maceration extract, 5g H-type ZSM-5 molecular sieves are added to maceration extract, 120 DEG C of oven dryings are positioned over after stirring
12h roasts 4h (heating rates at 500 DEG C:5 DEG C/min), after roasting through granulation, grind, be sized to 60-80 mesh to get negative
The MnZrSn/HZSM-5 catalyst of load type.
Embodiment 10
4.30g zirconium nitrates and 0.26g stannic chlorides are added in 2.86g manganese nitrate solutions (mass fraction 50%), stirred
It mixes to be uniformly mixed and is used as maceration extract, 3.33g H-type ZSM-5 molecular sieves are added to maceration extract, it is dry that 120 DEG C of baking ovens are positioned over after stirring
Dry 12h roasts 4h (heating rates at 500 DEG C:5 DEG C/min), after roasting through granulation, grind, be sized to 60-80 mesh to get
The MnZrSn/HZSM-5 catalyst of support type.
Application examples
Using toluene as VOCs model compounds, the low-temperature catalyzed oxygen that above-described embodiment obtains prepared catalyst is investigated
Change performance.Catalytic reaction condition is:Toluene concentration 1000ppm, catalyst amount 0.4g, reaction velocity 15,000mL/ (g h)
(referring to Fig. 1 and Fig. 2).
2,4,6 gained catalyst of embodiment shows good catalysis in toluene catalytic oxidation reaction as seen from Figure 1
Activity can convert completely in 250 DEG C of Toluenes, while 4 gained catalyst of embodiment has highest catalytic activity, 212
DEG C when toluene conversion be 50%, 235 DEG C of toluene conversions reach 100%, show that the catalyst has good low-temperature oxidation
Activity.
9 gained catalyst of embodiment has higher catalytic activity as seen from Figure 2, and at 275 DEG C, toluene can convert completely,
The complete conversion temperature of toluene of 7 gained catalyst of example is 285 DEG C, shows that H-type ZSM-5 molecular sieve is as carrier in the reaction
Effect is better than γ type aluminium oxide.
Embodiment described above is patent preferred application case of the present invention, but is not generated in any form to the present invention
Limitation.In actual application, without departing from the scope of the present invention, when in the technology using the disclosure above
Hold the equivalent embodiment made a little change or be modified to equivalent variations.
Claims (10)
1. a kind of volatile organic matter (VOCs) low-temperature catalytic oxidation catalyst, it is characterised in that:Catalyst activity component be manganese,
Zirconium and tin;Its molar ratio is followed successively by (0.60-0.90):(0.05-0.20):(0.05-0.20).
2. volatile organic matter low-temperature catalytic oxidation catalyst as described in claim 1, it is characterised in that:The catalyst is
Metal salt solution containing manganese, zirconium and tin is mixed with citric acid solution, is VOCs low-temperature oxidation catalytics after drying, roasting
Agent;Wherein, the molar ratio of citric acid and metal salt presoma is 0.8-1.4.
3. volatile organic matter low-temperature catalytic oxidation catalyst as described in claim 1, it is characterised in that:The catalyst is
Metal salt containing manganese, zirconium and tin is carried on carrier, wherein active component is that manganese, zirconium and tin molar ratio are followed successively by (0.60-
0.90):(0.05-0.20):(0.05-0.20), catalyst activity component load capacity is in terms of Mn elements, load capacity 0.01-
0.03mol Mn/10g carriers.
4. volatile organic matter low-temperature catalytic oxidation catalyst as described in claim 3, it is characterised in that:The catalyst is
To contain the metal salt of manganese, zirconium and tin as maceration extract, by carrier impregnation in wherein, and after after drying, roasting be support type
VOCs low-temperature oxidation catalysts.
5. by the volatile organic matter low-temperature catalytic oxidation catalyst described in claim 1-4 any one, it is characterised in that:Institute
It is manganese nitrate to state containing manganese Metal salt, is zirconium nitrate containing zirconium metal salt, is stannic chloride containing tin metal salt.
6. a kind of preparation method of volatile organic matter low-temperature catalytic oxidation catalyst described in claim 1, it is characterised in that:
1) manganese Metal salt, zirconium metal salt and tin metal salt are mixed according to aforementioned proportion with citric acid solution, is then stirred and evenly mixed
For use afterwards, citric acid is 0.8-1.4 with metal salt molar ratio
2) above-mentioned mixed solution under 60-80 DEG C of oil bath is stirred into 6-8h, is positioned over 100-120 DEG C of oven drying 12-20h,
400-600 DEG C of roasting 4-6h is gained catalyst after roasting.
7. a kind of preparation method of the volatile organic matter low-temperature catalytic oxidation catalyst described in claim 3, it is characterised in that:
It will contain manganese Metal salt, zirconium metal salt and tin metal mixed salt solution as maceration extract according to aforementioned proportion, be added to maceration extract
Carrier, it is gained catalysis after roasting that 100-120 DEG C of oven drying 12-20h, 400-600 DEG C of roasting 4-6h are positioned over after stirring
Agent;For catalyst activity component load capacity in terms of Mn elements, load capacity is 0.01-0.03mol Mn/10g carriers.
8. by the preparation method of the volatile organic matter low-temperature catalytic oxidation catalyst of claim 6 or 7, it is characterised in that:
The roasting roasts 4-6h with the heating rate of 5-8 DEG C/min at 400-600 DEG C, is granulated after roasting, grinds, is sized to 60-
80 mesh are to get catalyst.
9. by the preparation method of volatile organic matter low-temperature catalytic oxidation catalyst described in claim 7, it is characterised in that:It is described
Carrier is γ types aluminium oxide or H-type ZSM-5 molecular sieve.
10. a kind of application of volatile organic matter low-temperature catalytic oxidation catalyst described in claim 1, it is characterised in that:Institute
State catalysis material of the catalyst as light-concentration volatile organic exhaust gas catalytic purification.
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CN113996329A (en) * | 2021-11-08 | 2022-02-01 | 常州市恒纶纺织有限公司 | Catalyst for degrading VOCs (volatile organic compounds), and preparation method and application thereof |
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CN110075828A (en) * | 2019-06-06 | 2019-08-02 | 青岛大学 | A kind of preparation method of three-dimensional ordered macroporous structure manganese zirconium mixed oxide catalyst |
CN111558378A (en) * | 2019-10-28 | 2020-08-21 | 常州大学 | Catalytic degradation of toluene by Cu-Mn-CeO2 |
CN113996329A (en) * | 2021-11-08 | 2022-02-01 | 常州市恒纶纺织有限公司 | Catalyst for degrading VOCs (volatile organic compounds), and preparation method and application thereof |
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