CN106334565A - Composite air purification catalyst and preparation method thereof - Google Patents
Composite air purification catalyst and preparation method thereof Download PDFInfo
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- CN106334565A CN106334565A CN201610889910.9A CN201610889910A CN106334565A CN 106334565 A CN106334565 A CN 106334565A CN 201610889910 A CN201610889910 A CN 201610889910A CN 106334565 A CN106334565 A CN 106334565A
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- 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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- 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
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- 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
- B01D53/8671—Removing components of defined structure not provided for in B01D53/8603 - B01D53/8668
- B01D53/8675—Ozone
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- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/889—Manganese, technetium or rhenium
- B01J23/8892—Manganese
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Abstract
The invention discloses a composite air purification catalyst and a preparation method thereof. The composite air purification catalyst is prepared from manganese oxide composite copper oxide and cerium oxide. The preparation method comprises the steps that an oxidant, MnII salt, CuII salt and CeIII salt are dissolved in a solvent, the mixture is transferred to a high-pressure reaction kettle after mixing reaction, performs high temperature and high pressure reaction and then is filtered, cleaned and dried to obtain a composite catalyst precursor; the composite catalyst precursor is mixed with auxiliary materials and clay to get compound granulation powder; the compound granulation powder is granulated to obtain the composite air purification catalyst. The composite air purification catalyst prepared by adopting the preparation method is high in surface activity and high in catalytic performance.
Description
Technical field
The present invention relates to a kind of field of Environment Protection material, more particularly, to a kind of composite catalyst material for purification gas
Material.
Background technology
At present, facing mankind two large problems are environmental pollution and energy shortage, and wherein problem of environmental pollution is particularly pertinent.By
In in the last hundred years, create substantial amounts of bazardous waste during the development of mankind's modernization industry, environment is caused seriously
Pollution so that scope that in air, soil and water body, the content of pollutant can bear considerably beyond it.Compared to permissible
The soil being handled differently and water environment, the indoor air environment that atmospheric environment particularly people depend on for existence directly affects the mankind
Health, all-pervasive air pollutants have become as matter of utmost importance in need of immediate treatment.According to the difference of its form, air is dirty
Dye thing is broadly divided into particulate pollutant and volatile harmful gas pollutant, wherein volatile harmful gas pollutant essentially from
The tail gas producing in the vehicles such as waste gas, automobile and steamer produced by commercial production run and indoor hardware fitting and family
The volatile organic matter being given out in tool.
The harmful gass of in the air mainly have formaldehyde, ozone, benzene,toluene,xylene, carbon dioxide, nitrogen oxides, other
Multiple volatile harmful gas such as Organic substance, these harmful gass all endanger the health of the mankind to varying degrees.As formaldehyde
To Mucocutaneous stimulation, direct skin contact easily causes allergic inflammation even necrosis, and high-concentration formaldehyde can induce and prop up
San bronchial asthma even causes rhinopharyngeal neoplasm, or a kind of genotoxicity material.The respiratory tract of ozone meeting intense stimulus people, or even meeting
Cause human nerve to be poisoned, cause multiple diseases.Destroy the immune function of human body, induce lymphocyte chromosome pathological changes, accelerate
Aging, causes anemia of pregnant woman to have a deformed child.Volatile harmful gas (tvoc) is mostly irritant, causes immunity of organism off-leveling,
Impact central nervous system function, when serious can liver injury and hemopoietic system, moieties have been listed in carcinogen.
The mankind, in order to solve the pollution problem of in the air harmful gass, have carried out substantial amounts of research, create multiple air
Purification techniques.Earliest air clearing product carries out air cleaning using hepa drainage screen, and the granule being only capable of removing in the air is dirty
Dye thing, then helpless for hazardous air pollutants.The absorption of the inorganic porous materials such as activated carbon is applied empty in portioned product
Hazardous air pollutants in gas, can reduce the purpose of gas pollutant concentration.But adsorbing material is carrying out air
During purification, it is the specific surface area absorption harmful gass huge using it.After its surface excess reaches saturation, no
But cannot proceed to adsorb, and there is the risk that release causes secondary pollution, need to change adsorbing material.This purification
Material is unable to reach the purpose of thorough purification, needs periodic replacement absorption during the simply transfer of pollutant, and use
Material is it is difficult to meet the demand of harmful substance in purify air.At present, also create one kind for harmful gass in purify air
Photocatalyst technology, this technology adopt photocatalyst material as catalyst material, wherein photocatalyst catalyst material is mainly two
Titania meterial, under conditions of the irradiation of certain energy level light, using the hydroxyl free radical that the oxidability producing is extremely strong, catalysis
Decompose the poisonous and harmful substance of in the air, reach the purpose of purify air.This technology needs ability under specific illumination condition
Realize, cannot be using so that its application receives limitation in the environment of these conditions for providing；Additionally, its catalysis point
Solution is inefficient it is difficult to realization is widely applied.Additionally, noble metal has good catalytic performance, can effective catalytic decomposition
Harmful gass, yet with its application cost height it is difficult to realize large-scale application.
Numerous studies report surface, and transition metal oxide particularly Mn oxide has good catalysis activity, no
The effect playing spontaneous catalytic reaction in multiple reactions is can be implemented under the conditions of additional, and cheap, big rule can be met
The application of mould.However, during the carrying out of concrete catalytic reaction, the catalysis activity of catalyst is often subject to its internal crystal framework
The impact of structure, particle diameter, constituent, pattern and ambient conditions.The Mn oxide material of different crystalline lattice structure has different
Catalysis activity, after being doped with other metals with complementary and potentiation in its lattice structure, in catalytic reaction process
In can play coordinate catalysis effect, significantly improve the catalysis activity of catalyst material.The atom of these different metals is in chi
There is complementarity on very little and surface texture, therefore composite catalyst would generally be prepared into from multiple material doping, anti-in catalysis
Play synergism in answering, improve its catalytic performance；The self structure catalyst material different with pattern has different surfaces
Area and surface activity quantity, specific surface area is big, the catalyst material more than surface activity site can dramatically increase course of reaction
In effective collision number of times so that material possesses higher catalysis activity and catalytic decomposition efficiency；Application in catalyst material
During, add suitable adjuvant and can effectively improve its catalytic decomposition performance, good from surface property, absorption property is strong
Adjuvant, is distributed in the periphery in catalyst, can play the harmful gass adsorbing in the air in advance, increase active catalyst periphery
The effect of the concentration of harmful gass, effectively increases the Concentraton gradient of catalyst periphery harmful gass distribution, improves catalyst material
Catalytic decomposition efficiency.
A kind of nano titanium dioxide photocatalyst material for the voc that degrades is disclosed, preparation in cn 104174391 a
Nano titanium dioxide photocatalyst there is stronger visible absorption ability, relatively low electron-hole recombinations speed, can be fast
The benzene pollutant of fast completely degrading high concentration, only can be degradable little under visible light illumination in 4 hours with 0.1g mass
The benzene of low content in space.Wherein the quantity delivered of visible ray and absorbability are to govern its key to benzene catalytic decomposition performance
Factor, can speculate under the low light level or non-illuminated conditions, and its catalytic decomposition performance can substantially reduce or even lose efficacy it is impossible to expire comprehensively
The multiple region of foot or the demand of time period inner air-cleaning.Disclose for destroying co, voc and halogenation in cn 102481549 b
The oxidation catalyst of voc and method, describe one kind be deposited on suprabasil at a temperature of 250 DEG C to 450 DEG C destroy
The oxidation catalyst of the co in effluent streams and VOC, particularly halogenated organic compounds.Oxidation catalyst
Including at least two platinums group metal being supported on refractory oxide, one of which is platinum or ruthenium, described refractory oxide
For example, ceo2And zro2Solid solution and stannum oxide and/or silicon dioxide.Wherein select noble metal as active catalyst material
Material, high cost is difficult to apply on a large scale；In addition, this catalyst material need to carry out catalytic decomposition under hot conditionss more anti-
Should, high energy consumption, application cost height is it is difficult to be applied to common indoor air purification etc. cannot provide the field of hot environment.cn
A kind of preparation method of the catalyst of formaldehyde and ozone removal under room temperature is disclosed, using the oxidation in solution in 103506111 a
Reduction reaction is settled out presoma, obtains manganese dioxide-catalyst material in conjunction with calcine technology, at ambient temperature simultaneously by dirt
The harmful gass formaldehyde of dye in the air becomes harmless h with ozone decomposed2And co2, have no any harmful side product, go formaldehyde and
The advantage of ozone efficiency high.But its using the manganese dioxide-catalyst material that ordinary precipitation process obtains exist specific surface area low,
The low problem of show activity so that its purge amount relatively low it is difficult to meet the air that Current air pollution is complicated, pollutant load is high
The demand of environment inner air-cleaning.
In order to purify the air ambient that current contamination is serious and pollutant component is complicated, solve this global air dirty
Dye problem, urgent need one kind has degradation efficiency height concurrently, performance is good, can degrade multiple harmful gass, reusable and cost simultaneously
Cheap air cleaning catalyst material, for meeting air cleaning demand interior on a large scale.
Content of the invention
For above-mentioned involved problem, it is an object of the invention to provide a kind of air cleaning composite catalyst and its preparation
Method, described air cleaning catalytic composite material includes Mn oxide and is combined Cu oxide and cerium oxide.Described preparation side
In method, special reaction condition makes substantial amounts of cu2+And ce3+Enter into and in the middle of the microcosmic lattice structure of Mn oxide, replace manganese
Position obtains the composite catalyst presoma in the doping of lattice level, can play synergism；Add and there is bigger serface
Adjuvant as pelletize adjuvant, in conjunction with homogeneous mixed-forming technique, all effectively increasing air cleaning catalyst has in the air
The catalytic decomposition activity of evil material.
To achieve these goals, the present invention is to adopt the following technical scheme that a kind of air cleaning composite catalyst of realization
Preparation method, under the reaction condition of High Temperature High Pressure, process is doped to Mn oxide using copper and cerium, obtains doping type
Catalytic composite material.Choose oxidant, manganese salt, mantoquita and cerium salt mix at normal temperatures and carries out stirring reaction, higher in high temperature
Carry out recrystallization and impurity reaction under conditions of pressure, obtain the composite catalyst presoma with highly doped amount.Choose big
The inorganic porous material of specific surface area, as molding, granulating adjuvant, is uniformly mixed by homogeneous moulding process, purification efficiency
High air cleaning catalytic composite material.
This air cleaning catalytic composite material includes Mn oxide and is combined Cu oxide and cerium oxide.
The preparation technology of this air cleaning composite catalyst mainly includes the preparation of composite catalyst presoma and cladding is made
The process of grain.Specific as follows: air cleaning composite catalyst of the present invention is prepared via a method which: by oxidant, mnii
Salt, cuiiSalt and ceiiiSalt is dissolved in solvent and obtains mixed liquor, obtains precursor solution, by forerunner after being stirred reaction
Liquid solution refilters after high-temperature high-voltage reaction, cleans, being dried, and obtains powder composite catalyst presoma；Will be above-mentioned
Powder composite catalyst presoma is mixed homogeneously with adjuvant and clay and is obtained compound powder；By described compound powder
Air cleaning composite catalyst is obtained after forming processes.
Preferably, mn in Mn oxide, Cu oxide and cerium oxideii、cuiiAnd ceiiiMol ratio be (0.2-2)
: (0.05-1): (0.05-1), preferably (0.5-1.5): (0.05-0.5): (0.1-0.5).
Preferably, described air cleaning composite catalyst also includes adjuvant and clay, described adjuvant is selected inorganic porous
Material.
Preferably, described inorganic porous material include activated carbon, molecular sieve, silicon dioxide, silicon powder, titanium dioxide,
One or more of zeolite, aluminium oxide, attapulgite, meerschaum, Kaolin, montmorillonite, kieselguhr.
Preferably, described oxidant selects high manganese lithium, sodium permanganate, potassium permanganate, ammonium permanganate, perchloric acid,
Any one or more in Fenton reagent.
Preferably, described mniiSalt is selected any one in manganese sulfate, manganese nitrate, manganese carbonate, manganese chloride, manganese acetate
Plant or multiple.
Preferably, described cuiiAny one or more in copper sulfate, copper nitrate, copper chloride selected by salt.
Preferably, described ceiiiSalt is selected one or more in cerous nitrate, cerous sulfate, cerium chloride, ammonium ceric nitrate.
Preferably, oxidant, mniiSalt, cuiiSalt and ceiiiThe molar ratio of salt is (0.5-3): (0.2-2):
(0.05-1): (0.05-1), wherein it is preferably (1-2.5): (0.5-1.5): (0.05-0.5): (0.1-0.5).
Preferably, water selected by described solvent.
Preferably, oxidant, mn in described stirring reactioniiSalt, cuiiSalt and ceiiiFour kinds of solids of salt and solvent
Total solid-liquid specific mass is 1: (5-30), wherein preferably 1: (8-18).
Preferably, described stirring reaction temperature is 0-100 DEG C, wherein preferably 10-80 DEG C.
Preferably, the described stirring reaction time is 10-300min, preferably 20-180min.
Preferably, stir speed (S.S.) is 10-1000r/min, preferably 100-800r/min in described stirring reaction.
Preferably, described high-temperature high-voltage reaction temperature is 100-200 DEG C, preferably 120-190 DEG C.
Preferably, described high-temperature high-voltage reaction pressure is 0.3-3 MPa, wherein preferably 0.4-2 MPa.Above-mentioned
During high-temperature high-voltage reaction, solution temperature is higher, and the quantity of steam that it can send is more, and the pressure producing in reactor is also more
Greatly, in reactor solution can produce at different temperature with respect to high pressure.As under 190 DEG C of reaction condition, reactor
Interior pressure is 2 MPas, and under 100 DEG C of reaction condition, the pressure in reactor is 0.3 MPa.
Preferably, the described high-temperature high-voltage reaction time is 0.5-30h, wherein preferably 2-24h.
Preferably, described baking temperature is 60-300 DEG C, preferably 100-200 DEG C.
Preferably, described drying time is 3-30h, preferably 5-24h.
Preferably, inorganic porous material selected by described adjuvant, activated carbon, molecular sieve, silicon dioxide, silicon can be selected
One of micropowder, titanium dioxide, zeolite, alumina material, attapulgite, meerschaum, Kaolin, montmorillonite, kieselguhr or
Multiple.
Preferably, the particle size range of described clay is 200-600 mesh.
Preferably, the mixing quality of described composite catalyst presoma, adjuvant and clay is than for 1: (0.2-2):
(0.2-2), preferably 1: (0.5-1.5): (0.4-1.6).
Preferably, described forming processes comprise the steps: to add spheroidal particle seed in comminutor, turn certain
Speed is lower to add described binding agent and described compound powder, carries out pelletize and polishing obtains shaped granule, finally dry
Obtain spherical air cleaning composite catalyst.
Preferably, described spheroidal particle seed selects chemically inert inorganic material particle, such as aluminium oxide, oxidation
Silicon, calcium oxide and zirconium oxide.
Preferably, the particle size range of described spheroidal particle seed is 0.1-9mm, preferably 0.5-9mm.
Preferably, comminutor rotating speed is 10-60r/min, preferably 10-40r/min in described pelletize；
Preferably, the rotating speed of comminutor is 20-40r/min in described polishing；
Preferably, the time of described polishing is 10-100min.
Preferably, described forming processes comprise the steps: described compound powder and binding agent mix homogeneously,
And be added into stand-by in single lead screw ex truding briquetting machine material bin；Open single lead screw ex truding briquetting machine and carry out pelletize；Obtained granule is dried
Obtain spherical air cleaning composite catalyst.
Preferably, described binding agent selects one or more of water, nonpoisonous organic solvent, glue；
Preferably, the mass ratio of compound powder and binding agent is 1 in described granulation process: (0.2-1.2), excellent
Elect 1 as: (0.25-1.0)；
Preferably, described shaped granule drying temperature is 60-300 DEG C, preferably 100-200 DEG C；
Preferably, described shaped granule drying time is 1-30h, preferably 3-24h；
Preferably, described shaped granule diameter range is 0.2-10.2mm；
Described air cleaning composite catalyst apply indoors, formaldehyde, ozone and tvoc purification in in-car, cabin, cabin
On.
Compared with prior art, have the advantage that
1st, this nanoscale catalytic composite material surface activity high it is achieved that spontaneous in the case of no any additional condition
Carry out cartalytic decomposition effect；
2nd, adopt the manganese oxide catalyst material of high catalytic activity, can harmful gass effectively in purify air, and
Lossless during cartalytic decomposition effect, can reuse；
3rd, from having the doping component coordinating catalytic action, significantly improve the catalytic performance of catalyst material；
4th, carry out recrystallization reaction so that doping reaction is more abundant under high-temperature and high-pressure conditions；
5th, add the adjuvant of bigger serface, play the effect of absorption harmful gass, improve and have near catalyst material
The concentration of evil material, accelerates catalytic decomposition efficiency；
6th, use inorganic auxiliary material, while being effectively improved catalyst particle surface performance, having prevented granule makes for a long time
With during the phenomenon gone mouldy；
7th, polishing process effectively increases the surface property of granule.
Brief description
Fig. 1 is a sem figure of the composite catalyst presoma of the present invention.
Fig. 2 is the another sem figure of the composite catalyst presoma of the present invention.
Fig. 3 is the preparation technology flow chart of the air cleaning composite catalyst of the present invention.
Specific embodiment
With reference to the accompanying drawings the present invention is described more fully, the exemplary embodiment of the present invention is wherein described.
Embodiment 1
1708g pure water sequentially adds 39.5g potassium permanganate, 19.8g manganese chloride tetrahydrate, 12.5g copper sulphate pentahydrate and
13.6g six water cerous nitrate, stir to fully dispersed and dissolving after, blender rotating speed be 10r/min, at 0 DEG C react 300min.
Above-mentioned mixed solution is transferred in autoclave, under the conditions of being arranged on 150 DEG C reaction 16h after take out, cleaning, filter after
Dry 30h under the conditions of 60 DEG C, that is, obtain air cleaning composite catalyst presoma.
Above-mentioned composite catalyst presoma, silicon dioxide and clay are combined according to mass ratio 1: 2: 1 mix homogeneously
Pelletize powder is stand-by.The alumina particle choosing 0.1mm is added in granulating disc, and velocity of rotation is made for 60r/min
Grain, adopts in granulation process and uses water as binding agent, and wherein the interpolation mass ratio of compound powder and water is 1: 0.2, carries out
Granulation operations, when mean particle size reaches 0.2mm, stop charging, collect granule.The above-mentioned grain products collected are added
Enter and obtain shaped granule after being polished 10min in the granulating disc that rotating speed is 40r/min, take out and 3h is dried at 200 DEG C
Obtain air cleaning composite catalyst granule.
Test (being shown in Table 1) through bet, show that prepared composite catalyst presoma and composite catalyst specific grain surface amass
Larger.
Formaldehyde catalytic decomposition performance test: take the air cleaning composite catalyst granule of the above-mentioned preparation of 5.00g to be placed in diameter
Carry out catalytic decomposition activity assessment on core in the glass tubing of 10mm.The bottom of glass tubing is connected with formaldehyde generator, top
It is connected with gas chromatograph on-line detector.Air is squeezed in formaldehyde generator by pump and formaldehyde is mixed to get and containing concentration of formaldehyde is
The air of 1000ppm, air addition is 500ml/min, and the air containing formaldehyde enters the glass equipped with composite catalyst from bottom
In glass pipe, then the content entering into gas chromatograph on-line checking formaldehyde through glass tubing top.Testing result shows, the present embodiment
The air cleaning composite catalyst of middle preparation carries out catalytic decomposition to the formaldehyde of 1000ppm at ambient temperature, one-pass
Decomposition efficiency is 95%.
Catalytic decomposition of ozone performance test: assess air cleaning composite catalyzing using with above-mentioned test identical apparatus for evaluating
The decomposability to ozone for the agent granule, measures the concentration of ozone using ultraviolet spectrophotometer on-line detector.Method of testing is same
On, testing result shows, the air cleaning composite catalyst ozone to 120ppm at ambient temperature of preparation in the present embodiment
Carry out catalytic decomposition, its one-pass catalytic decomposition efficiency is shown in Table 2.
Tvoc gas purification performance test: assess air cleaning composite catalyzing using with above-mentioned test identical apparatus for evaluating
The decomposability to ozone for the agent granule, measures the concentration of tvoc using gas chromatograph.Method of testing ibid, testing result table
Bright, the air cleaning composite catalyst one-pass removal of tvoc to 400ppm at ambient temperature of preparation in the present embodiment
Efficiency is shown in Table 2.
Benzene, toluene and the test of dimethylbenzene purifying property: choose temperature and be 23-27 DEG C, a size of 30m3Test chamber environment
Inside carry out the air cleaning performance evaluation of this multifunctional air purifying catalytic composite material.Choose benzene, toluene and dimethylbenzene this
Three kinds of harmful substances carry out test event for clean-up effect.Find through detection, prepared multi-functional air in the present embodiment
Purify catalytic composite material and 2 are shown in Table to the 1h purifying rate of benzene, toluene and dimethylbenzene.
Embodiment 2
28g potassium permanganate, 28.7g six water manganese nitrate, 8.5g copper chloride dihydrate and 17.7g is sequentially added in 786g pure water
Six water cerium chlorides, stir to fully dispersed and dissolving after, blender rotating speed be 1000r/min, at 100 DEG C react 10min.Will
Above-mentioned mixed solution is transferred in autoclave, under the conditions of being arranged on 100 DEG C reaction 30h after take out, cleaning, filter after
Dry 2h under the conditions of 200 DEG C, that is, obtain air cleaning composite catalyst presoma.
Above-mentioned composite catalyst presoma, silicon powder and clay are combined according to mass ratio 1: 0.5: 2 mix homogeneously
Pelletize powder is stand-by.The silica dioxide granule choosing 0.2mm is added in granulating disc, and velocity of rotation is carried out for 45r/min
Pelletize, adopts in granulation process and uses water as binding agent, and wherein the interpolation mass ratio of compound powder and water is 1: 0.3, enters
Row granulation operations, when mean particle size reaches 2mm, stop charging, collect granule.The above-mentioned grain products collected are added
Enter and obtain shaped granule after being polished 50min in the roller drier that rotating speed is 30r/min, take out and 10h is dried at 150 DEG C
Obtain air cleaning composite catalyst granule.
Test (being shown in Table 1) through bet, show that prepared composite catalyst presoma and composite catalyst specific grain surface amass
Larger.
With embodiment 1, its testing result is shown in Table 2 to particulates' properties method of testing.
Embodiment 3
285g pure water sequentially adds 31.6g potassium permanganate, 17.8g tetra- water manganese sulfate, 1.2g nitrate trihydrate copper and
6.4g tetra- water cerous sulfate, stir to fully dispersed and dissolving after, blender rotating speed be 150r/min, at 20 DEG C react
180min.Above-mentioned mixed solution is transferred in autoclave, takes out after reaction 2h under the conditions of being arranged on 180 DEG C, cleaning, mistake
Filter dries 20h under the conditions of 100 DEG C, that is, obtain air cleaning composite catalyst presoma.
Above-mentioned composite catalyst presoma, kieselguhr and clay are combined according to mass ratio 1: 0.2: 1 mix homogeneously
Pelletize powder is stand-by.The zirconia particles choosing 0.2mm are added in granulating disc, and velocity of rotation is made for 10r/min
Grain, adopts in granulation process and uses water as binding agent, and wherein the interpolation mass ratio of compound powder and water is 1: 0.45, carries out
Granulation operations, when mean particle size reaches 1mm, stop charging, collect granule.The above-mentioned grain products collected are added
Rotating speed obtains shaped granule after being polished 30min in the roller drier for 20r/min, taking-up is dried 5h at 180 DEG C and is
Obtain air cleaning composite catalyst granule.
Test (being shown in Table 1) through bet, show that prepared composite catalyst presoma and composite catalyst specific grain surface amass
Larger.
With embodiment 1, its testing result is shown in Table 2 to particulates' properties method of testing.
Embodiment 4
1470g pure water sequentially adds 223.7g potassium permanganate, 17.2g six water manganese nitrate, 7.3g nitrate trihydrate copper and
10.6g six water cerium chloride, stir to fully dispersed and dissolving after, blender rotating speed be 800r/min, at 80 DEG C react
50min.Above-mentioned mixed solution is transferred in autoclave, takes out after reaction 0.5h under the conditions of being arranged on 200 DEG C, cleaning,
Filter and dry 15h under the conditions of 120 DEG C, that is, obtain air cleaning composite catalyst presoma.
Above-mentioned composite catalyst presoma, aluminium oxide and clay are answered according to mass ratio 1: 0.8: 0.2 mix homogeneously
Close pelletize powder stand-by.The alumina particle choosing 0.4mm is added in granulating disc, and velocity of rotation is carried out for 20r/min
Pelletize, adopts in granulation process and uses water as binding agent, and wherein the interpolation mass ratio of compound powder and water is 1: 0.4, enters
Row granulation operations, when mean particle size reaches 5mm, stop charging, collect granule.The above-mentioned grain products collected are added
Enter and obtain shaped granule after being polished 80min in the roller drier that rotating speed is 25r/min, take out and 30h is dried at 60 DEG C
Obtain air cleaning composite catalyst granule.
Test (being shown in Table 1) through bet, show that prepared composite catalyst presoma and composite catalyst specific grain surface amass
Larger.
With embodiment 1, its testing result is shown in Table 2 to particulates' properties method of testing.
Embodiment 5
2145g pure water sequentially adds 28.4g potassium permanganate, 20.1g six water manganese nitrate, 10.2g copper chloride dihydrate and
12.8g tetra- water cerous sulfate, stir to fully dispersed and dissolving after, blender rotating speed be 300r/min, at 60 DEG C react
100min.Above-mentioned mixed solution is transferred in autoclave, takes out after reaction 15h under the conditions of being arranged on 120 DEG C, cleaning,
Filter and dry 10h under the conditions of 150 DEG C, that is, obtain air cleaning composite catalyst presoma.
Above-mentioned composite catalyst presoma, activated carbon and clay are combined according to mass ratio 1: 1: 0.5 mix homogeneously
Pelletize powder is stand-by.The alumina particle choosing 9mm is added in granulating disc, and velocity of rotation carries out pelletize for 30r/min,
Granulation process is adopted and uses water as binding agent, wherein the interpolation mass ratio of compound powder and water is 1: 0.35, is made
Grain operation, when mean particle size reaches 10mm, stops charging, collects granule.The above-mentioned grain products collected are added
Rotating speed obtains shaped granule after being polished 100min in the roller drier for 35r/min, takes out and 15h is dried at 120 DEG C
Obtain air cleaning composite catalyst granule.
Test (being shown in Table 1) through bet, show that prepared composite catalyst presoma and composite catalyst specific grain surface amass
Larger.
With embodiment 1, its testing result is shown in Table 2 to particulates' properties method of testing.
Comparative example 1 (no high-temperature high-voltage reaction process)
1708g pure water sequentially adds 39.5g potassium permanganate, 19.8g manganese chloride tetrahydrate, 12.5g copper sulphate pentahydrate and
13.6g six water cerous nitrate, stir to fully dispersed and dissolving after, blender rotating speed be 10r/min, at 0 DEG C react 300min
Afterwards, cleaning, filtration dry 30h under the conditions of 60 DEG C, that is, obtain air cleaning composite catalyst presoma.
Above-mentioned composite catalyst presoma, silicon dioxide and clay are combined according to mass ratio 1: 2: 1 mix homogeneously
Pelletize powder is stand-by.The alumina particle choosing 0.1mm is added in granulating disc, and velocity of rotation is made for 60r/min
Grain, adopts in granulation process and uses water as binding agent, and wherein the interpolation mass ratio of compound powder and water is 1: 0.2, carries out
Granulation operations, when mean particle size reaches 0.2mm, stop charging, collect granule.The above-mentioned grain products collected are added
Enter and obtain shaped granule after being polished 10min in the roller drier that rotating speed is 40r/min, take out and 1h is dried at 200 DEG C
Obtain air cleaning composite catalyst granule.
Test (being shown in Table 1) through bet, show that prepared composite catalyst presoma and composite catalyst specific grain surface amass
Less.
With embodiment 1, its testing result is shown in Table 2 to particulates' properties method of testing.
Comparative example 2 (non-impurity-doped composition)
Sequentially add 39.5g potassium permanganate and 19.8g manganese chloride tetrahydrate in 1708g pure water, stir to fully dispersed and
After dissolving, blender rotating speed is 10r/min, reacts 300min at 0 DEG C.Above-mentioned mixed solution is transferred to autoclave
In, take out after reaction 16h under the conditions of being arranged on 150 DEG C, cleaning, filtration dry 30h under the conditions of 60 DEG C, that is, obtain air net
Change composite catalyst presoma.
Above-mentioned composite catalyst presoma, silicon dioxide and clay are combined according to mass ratio 1: 2: 1 mix homogeneously
Pelletize powder is stand-by.The alumina particle choosing 0.1mm is added in granulating disc, and velocity of rotation is made for 60r/min
Grain, adopts in granulation process and uses water as binding agent, and wherein the interpolation mass ratio of compound powder and water is 1: 0.2, carries out
Granulation operations, when mean particle size reaches 0.2mm, stop charging, collect granule.The above-mentioned grain products collected are added
Enter and obtain shaped granule after being polished 10min in the roller drier that rotating speed is 40r/min, take out and lh is dried at 200 DEG C
Obtain air cleaning composite catalyst granule.
Test (being shown in Table 1) through bet, show that prepared composite catalyst presoma and composite catalyst specific grain surface amass
Larger.
With embodiment 1, its testing result is shown in Table 2 to particulates' properties method of testing.
Comparative example 3 (granulation process no adjuvant adds)
1708g pure water sequentially adds 39.5g potassium permanganate, 19.8g manganese chloride tetrahydrate, 12.5g copper sulphate pentahydrate and
13.6g six water cerous nitrate, stir to fully dispersed and dissolving after, blender rotating speed be 10r/min, at 0 DEG C react 300min.
Above-mentioned mixed solution is transferred in autoclave, under the conditions of being arranged on 150 DEG C reaction 16h after take out, cleaning, filter after
Dry 30h under the conditions of 60 DEG C, that is, obtain air cleaning composite catalyst presoma.
Above-mentioned composite catalyst presoma and clay are obtained compound powder according to mass ratio 1: 1 mix homogeneously treat
With.The alumina particle choosing 0.1mm is added in granulating disc, and velocity of rotation carries out pelletize for 60r/min, in pelletize
Adopt in journey and use water as binding agent, wherein the interpolation mass ratio of composite catalyst presoma and water is 1: 0.2, carries out pelletize behaviour
Make, when mean particle size reaches 0.2mm, stop charging, collect granule.The above-mentioned grain products collected are added rotating speed
For being polished after 10min obtaining shaped granule in the granulating disc of 40r/min, taking-up is dried 3h at 200 DEG C and obtains
Air cleaning composite catalyst granule.
Test (being shown in Table 1) through bet, show that prepared composite catalyst presoma and composite catalyst specific grain surface amass
Less.
With embodiment 1, its testing result is shown in Table 2 to particulates' properties method of testing.
Comparative example 4 (material proportion comparative example)
2145g pure water sequentially adds 1.58g potassium permanganate, 20.1g six water manganese nitrate, 10.2g copper chloride dihydrate and
12.8g tetra- water cerous sulfate, the solid-to-liquid ratio of its reaction mass is 1: 36, stirs to fully dispersed and dissolving, blender rotating speed is
300r/min, reacts 100min at 60 DEG C.Above-mentioned mixed solution is transferred in autoclave, is arranged on 120 DEG C of conditions
Take out after lower reaction 15h, cleaning, filtration dry 10h under the conditions of 150 DEG C, that is, obtain air cleaning composite catalyst forerunner
Body.
Above-mentioned composite catalyst presoma, activated carbon and clay are combined according to mass ratio 1: 1: 0.5 mix homogeneously
Pelletize powder is stand-by.The alumina particle choosing 9mm is added in granulating disc, and velocity of rotation carries out pelletize for 30r/min,
Granulation process is adopted and uses water as binding agent, wherein the interpolation mass ratio of compound powder and water is 1: 0.35, is made
Grain operation, when mean particle size reaches 10mm, stops charging, collects granule.The above-mentioned grain products collected are added
Rotating speed obtains shaped granule after being polished 100min in the roller drier for 35r/min, takes out and 15h is dried at 120 DEG C
Obtain air cleaning composite catalyst granule.
Test (being shown in Table 1) through bet, show that prepared composite catalyst presoma and composite catalyst specific grain surface amass
Larger.
With embodiment 1, its testing result is shown in Table 2 to particulates' properties method of testing.
Comparative example 5 (material proportion comparative example)
2145g pure water sequentially adds 28.4g potassium permanganate, 20.1g six water manganese nitrate, 0.17g copper chloride dihydrate and
12.8g tetra- water cerous sulfate, the solid-to-liquid ratio of its reaction mass is 1: 36, stirs to fully dispersed and dissolving, blender rotating speed is
300r/min, reacts 100min at 60 DEG C.Above-mentioned mixed solution is transferred in autoclave, is arranged on 120 DEG C of conditions
Take out after lower reaction 15h, cleaning, filtration dry 10h under the conditions of 150 DEG C, that is, obtain air cleaning composite catalyst forerunner
Body.
Above-mentioned composite catalyst presoma, activated carbon and clay are combined according to mass ratio 1: 1: 0.5 mix homogeneously
Pelletize powder is stand-by.The alumina particle choosing 9mm is added in granulating disc, and velocity of rotation carries out pelletize for 30r/min,
Granulation process is adopted and uses water as binding agent, wherein the interpolation mass ratio of compound powder and water is 1: 0.35, is made
Grain operation, when mean particle size reaches 10mm, stops charging, collects granule.The above-mentioned grain products collected are added
Rotating speed obtains shaped granule after being polished 100min in the roller drier for 35r/min, takes out and 15h is dried at 120 DEG C
Obtain air cleaning composite catalyst granule.
Test (being shown in Table 1) through bet, show that prepared composite catalyst presoma and composite catalyst specific grain surface amass
Larger.
With embodiment 1, its testing result is shown in Table 2 to particulates' properties method of testing.
Table 1: the specific surface area table of composite catalyst presoma and composite catalyst granule
Table 2: composite catalyst Particulate Air purifying property testing result table
| Sample | Formaldehyde | Ozone | tvoc | Benzene | Toluene | Dimethylbenzene |
| Embodiment 1 | 95% | 95% | 98% | 99% | 99% | 99% |
| Embodiment 2 | 93% | 91% | 98% | 99% | 98% | 99% |
| Embodiment 3 | 91% | 88% | 99% | 98% | 99% | 97% |
| Embodiment 4 | 88% | 92% | 99% | 96% | 98% | 99% |
| Embodiment 5 | 90% | 86% | 97% | 99% | 96% | 99% |
| Comparative example 1 | 24% | 17% | 21% | 26% | 27% | 22% |
| Comparative example 2 | 40% | 23% | 20% | 28% | 29% | 30% |
| Comparative example 3 | 46% | 52% | 47% | 57% | 53% | 61% |
| Comparative example 4 | 16% | 9% | 23% | 19% | 16% | 21% |
| Comparative example 5 | 62% | 59% | 67% | 56% | 51% | 68% |
Above content is only presently preferred embodiments of the present invention, for those of ordinary skill in the art, according to the present invention's
Thought, all will change in specific embodiments and applications, and this specification content should not be construed as to the present invention
Restriction.
Claims (10)
1. a kind of air cleaning composite catalyst is it is characterised in that described air cleaning catalytic composite material includes manganese oxidation
Thing is combined Cu oxide and cerium oxide.
2. air cleaning composite catalyst according to claim 1, wherein, Mn oxide, Cu oxide and cerium oxide
Middle mnii、cuiiAnd ceiiiMol ratio be (0.2-2): (0.05-1): (0.05-1), preferably (0.5-1.5): (0.05-
0.5)∶(0.1-0.5).
3. air cleaning composite catalyst according to claim 1 and 2, wherein, described air cleaning composite catalyst is also
Including adjuvant and clay, inorganic porous material selected by described adjuvant.
4. air cleaning composite catalyst according to claim 3, wherein, described inorganic porous material include activated carbon,
In molecular sieve, silicon dioxide, titanium dioxide, zeolite, aluminium oxide, attapulgite, meerschaum, Kaolin, montmorillonite, kieselguhr
One or more.
5. a kind of preparation method of the air cleaning composite catalyzing described in any one of claim 1-4, comprises the steps:
By oxidant, mniiSalt, cuiiSalt and ceiiiSalt is dissolved in solvent and obtains mixed liquor, before obtaining after being stirred reaction
Drive liquid solution, described precursor solution is refiltered after high-temperature high-voltage reaction, cleans, is dried, obtain powder and be combined
Catalyst precursor；
Described powder composite catalyst presoma is mixed homogeneously with adjuvant and clay and obtains compound powder；
Described compound raw material is obtained described air cleaning composite catalyst after forming processes.
6. the preparation method of air cleaning composite catalyst according to claim 5, wherein, described oxidant is from high
LiMn2O4, sodium permanganate, potassium permanganate, ammonium permanganate, perchloric acid, any one or more in Fenton reagent.
7. the preparation method of the air cleaning composite catalyst according to claim 5 or 6, wherein, described mniiSulfur selected by salt
Any one or more in sour manganese, manganese nitrate, manganese carbonate, manganese chloride, manganese acetate.
8. the preparation method of the air cleaning composite catalyst according to any one of claim 5-7, wherein, described cuii
Any one or more in copper sulfate, copper nitrate, copper chloride selected by salt.
9. the preparation method of the air cleaning composite catalyst according to any one of claim 5-8, wherein, described ceiiiSalt
From one or more in cerous nitrate, cerous sulfate, cerium chloride, ammonium ceric nitrate.
10. the preparation method of the air cleaning composite catalyst according to any one of claim 5-9, wherein, oxidant,
mniiSalt, cuiiSalt and ceiiiThe molar ratio of salt is (0.5-3): (0.2-2): (0.05-1): (0.05-1), wherein preferably
For (1-2.5): (0.5-1.5): (0.05-0.5): (0.1-0.5).
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| CN119236873B (en) * | 2024-11-07 | 2025-05-13 | 稀瑞材料技术(杭州)有限公司 | Composite purifying material and preparation method thereof |
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| CN106334565B (en) | 2020-06-09 |
| WO2018068729A1 (en) | 2018-04-19 |
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