CN107321148A - A kind of VOCs for removing low concentration big flow method and its modified catalyst - Google Patents
A kind of VOCs for removing low concentration big flow method and its modified catalyst Download PDFInfo
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- 238000000034 method Methods 0.000 title claims abstract description 48
- 239000012855 volatile organic compound Substances 0.000 title claims abstract description 24
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- 229910052723 transition metal Inorganic materials 0.000 claims abstract description 10
- 150000003624 transition metals Chemical class 0.000 claims abstract description 10
- 238000012545 processing Methods 0.000 claims abstract description 6
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 100
- 230000001413 cellular effect Effects 0.000 claims description 37
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 claims description 26
- VQWQYXBWRCCZGX-UHFFFAOYSA-N acetic acid;manganese Chemical compound [Mn].CC(O)=O.CC(O)=O VQWQYXBWRCCZGX-UHFFFAOYSA-N 0.000 claims description 23
- 239000000203 mixture Substances 0.000 claims description 21
- 238000006243 chemical reaction Methods 0.000 claims description 20
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- 238000001035 drying Methods 0.000 claims description 7
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- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 52
- 239000002912 waste gas Substances 0.000 description 25
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- 241000256844 Apis mellifera Species 0.000 description 3
- 229910016978 MnOx Inorganic materials 0.000 description 3
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 3
- 239000003463 adsorbent Substances 0.000 description 3
- 239000000443 aerosol Substances 0.000 description 3
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- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000004411 aluminium Substances 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000001580 bacterial effect Effects 0.000 description 1
- 230000033558 biomineral tissue development Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000009841 combustion method Methods 0.000 description 1
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Classifications
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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
- B01D53/75—Multi-step processes
-
- 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
- B01D53/38—Removing components of undefined structure
- B01D53/44—Organic components
-
- 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
- B01D53/8671—Removing components of defined structure not provided for in B01D53/8603 - B01D53/8668
- B01D53/8675—Ozone
-
- 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
- B01D53/8678—Removing components of undefined structure
- B01D53/8687—Organic components
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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
-
- 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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
- B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
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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
- B01D2257/708—Volatile organic compounds V.O.C.'s
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2259/00—Type of treatment
- B01D2259/80—Employing electric, magnetic, electromagnetic or wave energy, or particle radiation
- B01D2259/818—Employing electrical discharges or the generation of a plasma
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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Abstract
The invention discloses a kind of low-temperature plasma synergistic modified two sections of removing VOCs of catalyst method, CO2 and H that organic exhaust gas is produced after the processing of efficient plasma reactor2O and bag accessory substance ozoniferous etc. are passed through the catalyst being modified by charing pretreatment and containing transition metal, and the accessory substance is converted by catalysed oxidn, complete the harmless treatment to VOCs.The method for preparing catalyst is simple, and cheap, binding plasma reactor greatly reduces energy consumption, is adapted to industrial applications.
Description
Technical field
The invention belongs to VOC (VOCs) removing sulfuldioxide field, and in particular to a kind of low temperature plasma association
With catalytic treatment VOCs technique.
Background technology
In recent years, the multiple cities of China occurred in that large-scale haze weather, and the duration is longer, and haze essence is just
Be atmospheric aerosol concentration be in higher level.And Organic aerosol is one of main component in atmospheric aerosol, in mist
The serious regional Organic aerosol of haze typically constitutes from PM10And PM2.5The 20-60% of quality.And formed Organic aerosol it is important before
It is exactly volatile organic matter to drive thing.As things go, the typical industry VOCs discharges environmental pollution of China is very serious,
And have the trend of sustainable growth, therefore VOCs emission control is not allowed to delay.
General VOCs control technology is divided into process control and the major class of end treatment two, but is due to current scientific and technical water
Flat limitation, process control is difficult to sometimes, must just use end-of-pipe control technology, and the most of processing skills used now
Art is all end treatment, mainly including absorption process, absorption method, condensation method, combustion method, catalytic oxidation, bioanalysis etc..It is several recently
Comparison on plasma body cooperative technical research in 10 years is more, and many scholars are had found in actual applications, with conventional purge technology
The low temperature plasma catalysis technique that compares has advantages below：Normal-temperature reaction is easy-to-use without heating, and greatly saves
The about energy.
Plasma is used alone and removes organic exhaust gas, high energy consumption is often encountered and the problem of accessory substance is difficult to control to；
Concentration, secondary pollution and costly limitation are frequently subjected to again if only organic exhaust gas is removed using other conventional arts.
According to the experimental study of scholars before, it was demonstrated that waited gas ions to be used in combination to produce with conventional art and significantly cooperate with work
With.Mainly there are plasma combination absorption method, plasma combined catalyst method, plasma combination bioanalysis etc., wherein closing
It is more deep with the technical research that adsorbent is combined in plasma.The modification of adsorbent species, adsorbent is related generally to, it is dense
The influence to synergistic purification technology such as degree, voltage, and further study the generation for how suppressing accessory substance.
Such as Wang Xiangqian delivered in 2015 it is entitled " dielectric barrier discharge coupled biological drop filter purification multicomponent VOCs's
Existing various VOCS processing methods are inquired into key technology and technical study ", sum up grade as shown in table 1 from
Daughter Research progress, it is seen then that prior art can realize that the 100% of pollutant removes, but its corresponding CO2Selectivity
Only 80-85%, and not up to permineralization level, although can improve mineralization rate using transition-metal catalyst, but instead
The accumulation that the accessory substances such as carbon black pellet are still had inside device is answered, even if reducing carbon black pellet with reference to Pt, Pd Precious metal oxidation aluminium,
Gaseous by-product can be still produced, the problem of existing in face of prior art, Wang Xiangqian utilizes a kind of bacterium of efficient degradation dimethylbenzene
Strain, VOCs removal is realized in conjunction with dielectric barrier discharge, although this method effect is good, is operated complex, it is necessary to raw
Thing bacterial strain is just achieved.
The research of the dielectric barrier discharge technology of table 1 and collaboration PROCESS FOR TREATMENT VOC
The content of the invention
Conversion ratio is low during for solution prior art progress VOCs processing, the problem of being also easy to produce accessory substance, complex operation, this hair
The bright one kind that provides can just remove low concentration big flow VOCs merely with two steps of low temperature plasma and modified catalyst
Method, this method effectively increases VOCs removal efficiency, reduces the discharge of accessory substance, reduces the energy consumption of reaction.
To realize the technical purpose of the present invention, one aspect of the present invention provides a kind of VOCs's for removing low concentration big flow
Method, it is characterised in that including：
Steam is passed into the internal reaction of low temperature plasma provided with the metal electrode being fixed in dielectric in advance
In device, make to produce that enough being reacted with other free radicals to form stationary atom or molecule includes OH in the reactor
Active particle；
Volatile organic matter is passed through into the reactor for generating active particle, it is described under high-tension current effect
Volatile organic matter is degraded, and is produced and is included CO2、H2O and accessory substance ozone mixture；
The mixture is adsorbed and catalysis oxidation using modified catalyst, the ozone in the mixture is inhaled
Attached conversion, volatile organic matter is removed.
Wherein, the modified catalyst is by charing pretreatment and the modified cellular activated carbon of containing transition metal.
Wherein, the weight part ratio of the steam and volatile organic matter is 10-20:80-90.
Preferably, the weight part ratio of the steam and volatile organic matter is 16:84.
Wherein, the metal electrode is stainless steel bar, and the dielectric is quartz glass, and the low temperature plasma is anti-
It is spool formula dielectric impedance reactor to answer device.
Wherein, the applied voltage for producing high-tension current is 16.8-18.0kV, and discharge power is 140-155w.
Preferably, the applied voltage for producing high-tension current is 17-17.5kV, and discharge power is 140-150w
Wherein, the modified catalyst is by charing pretreatment and the modified cellular activated carbon of containing transition metal.
Wherein, mass percent of the transition metal in modified activated carbon is 1-7%.
Particularly, the transition metal is Mn.
To realize the technical purpose of the present invention, further aspect of the present invention provides a kind of Modified catalytic for being used to remove VOCs
Agent, it is, by charing pretreatment and the modified cellular activated carbon of containing transition metal, to be prepared by following steps：
Cellular activated carbon is subjected to charing pretreatment under nitrogen atmosphere；
Pretreated cellular activated carbon will be carbonized and be immersed in acetic acid manganese solution, acetic acid manganese solution is fully penetrated into honeycomb
In activated carbon；
The cellular activated carbon for being impregnated with acetic acid manganese solution is dried after processing, dried cellular activated carbon is obtained；
The cellular activated carbon of the acquisition is subjected to calcination process in nitrogen atmosphere, modified catalyst is obtained.
Wherein, the drying process is to dry the acetic acid manganese solution for being impregnated with cellular activated carbon in air dry oven
It is dry.
Wherein, the temperature of the charing pretreatment is 500 DEG C -900 DEG C.
Wherein, the drying process temperature is 60-100 DEG C, and drying time period is 10-14h.
Preferably, the drying process temperature is 80 DEG C, and drying time period is 12h.
Wherein, the calcination process temperature is 300-600 DEG C, roasting duration 1.5-3.5h.
Preferably, the calcination process temperature is 400-500 DEG C, roasting duration 2h.
The present invention also provide it is a kind of by above-mentioned modified catalyst be used for handle reaction of low temperature plasma device degraded VOCs
The purposes of the mixture of the accessory substance of produced ozone afterwards.
Compared with prior art, the advantages of the present invention are：
(1) present invention is plasma technique, absorption and the effective integration of catalysis technique technique, plays three kinds of technologies each
, can be disposably while the efficient a variety of VOCs for eliminating various concentrations while the feature of kind, moreover it is possible to produce effective synergy.
(2) present invention is applied to low concentration, atm number, the processing of the organic exhaust gas of complicated component.
(3) 16% steam that the present invention is passed through in advance produces active group, OH increase in the presence of high energy electron
So that the removal efficiency of organic exhaust gas is improved.
(4) the modified catalyst of the present invention can improve the decomposition of ozone, reduce the generation of accessory substance.
(6) catalyst prepared by the present invention can carry out plasma-catalytic concerted reaction, energy consumption reduction, price at normal temperatures
Cheap suitable commercial Application.
Brief description of the drawings
Fig. 1 is the removal efficiency effect line chart of test example 1 of the present invention；
Fig. 2 is the removal efficiency effect line chart of test example 2 of the present invention；
Fig. 3 is that the removal efficiency effect of test example 3 of the present invention compares line chart.
In figure, Mn/AC-A represents the activated carbon being modified by manganese Metal.
Embodiment
With reference to specific embodiment, the present invention is expanded on further.But these embodiments be only limitted to explanation the present invention without
For limiting the scope of the present invention.The experimental method of unreceipted specific experiment condition in the following example, generally according to conventional strip
Part, or according to the condition proposed by manufacturer.
Embodiment 1
1st, the preparation of modified catalyst
Commercially available cellular activated carbon is subjected to charing pretreatment at 800 DEG C, charing pre-treatment step is using conventional behaviour
Make technology, the mass fraction that then adulterates is modified for 3% manganese oxide, and doping process is to claim the cellular activated carbon after charing
Be impregnated into respectively after amount in the acetic acid manganese solution configured, impregnate 24h, after the completion of 12h is dried in 80 DEG C of air dry ovens, dry
After place into retort 300 DEG C of roasting temperatures under nitrogen atmosphere, under the high temperature conditions, acetic acid manganese solution is in honeycomb activity
Carbon surface formation manganese oxide, obtains modified catalyst, wherein, the mass fraction of manganese oxide is 3%.
2nd, degradation treatment
Steam is passed into reaction of low temperature plasma device in advance, after energization, electrion makes steam in the reactor
Produce enough free radical activity particles, such as OH, O, HO2, while low temperature plasma can also produce the O of strong oxidizing property3, so
Xylene waste gas is passed into plasma reactor again afterwards, wherein, the volumetric usage ratio of steam and dimethylbenzene is:17：83,
Lasting electrion makes the free radicals of enough strong oxidizing properties be reacted with dimethylbenzene, make the chemical bond rupture of dimethylbenzene from
Solution, last dimethylbenzene is degraded into CO2、H2The mixture such as O and accessory substance, also obtains the harmful substance-smelly of low temperature plasma generation
Oxygen；Wherein, the applied voltage of plasma reactor is 17.3kV, and the discharge power of plasma is 142.5w, gas (i.e. two
Toluene waste gas) flow velocity be 150L/h, dimethylbenzene initial concentration be 137ppm, air speed (GHSV) be 10000h-1。
It should be noted that metal electrode used in the present invention is stainless steel bar, dielectric is quartz glass, low temperature
Plasma reactor is that spool formula dielectric impedance reactor is obtained by commercially available.
3rd, absorption and catalytic treatment
At ambient temperature, mixture step 2 degraded is sent to the modified catalyst prepared equipped with step 1 with ozone
Hydrogen-catalyst reactor in, in the presence of cellular activated carbon, on activated carbon active sites to ozone carry out adsorption-decomposition function, simultaneously bear
Ozone is catalytically decomposed the MnOx for being loaded in activated carbon surface, the Mn of MnOx surface exposuresn+Ion, O2 2-, different oxidation state
Defective bit, unsaturated coordination valence and acid activated centre, MnOx and O can be made3Reaction, and promote it to O2Conversion, CO2、
H2O and accessory substance are removed and mineralising；Wherein, catalyst amount is 5.5g, and volume is about 15cm3, under normal temperature condition, to most
Dimethylbenzene, the ozone obtained eventually in product is detected, obtains testing result as shown in table 2.
It should be noted that the room temperature condition described in the present invention is any temperature in the range of 25-35 DEG C, such as 26 DEG C,
27 DEG C, 28 DEG C, 29 DEG C, 30 DEG C, 31 DEG C, 32 DEG C, 33 DEG C, 34 DEG C etc..
Embodiment 2
1st, the preparation of modified catalyst
Commercially available cellular activated carbon is subjected to charing pretreatment at 500 DEG C, charing pre-treatment step is using conventional behaviour
Make technology, the mass fraction that then adulterates is modified for 1% manganese oxide, and doping process is to claim the cellular activated carbon after charing
Be impregnated into respectively after amount in the acetic acid manganese solution configured, impregnate 30h, after the completion of 14h is dried in 60 DEG C of air dry ovens, dry
After place into retort 300 DEG C of roasting temperatures under nitrogen atmosphere, under the high temperature conditions, acetic acid manganese solution is lived in honeycomb
Property carbon surface formation manganese oxide, obtain modified catalyst, wherein, the mass fraction of manganese oxide is 1%.
2nd, degradation treatment
Steam is passed into reaction of low temperature plasma device in advance, xylene waste gas is then passed into plasma again
Reactor, wherein, the volume ratio of steam and dimethylbenzene is 4:21, last dimethylbenzene is degraded into CO2、H2O and accessory substance etc. are mixed
Thing, also obtains harmful substance-ozone of low temperature plasma generation；Wherein, the applied voltage of plasma reactor is
16.9kV, the discharge power of plasma is 140.0w, and gas (i.e. xylene waste gas) flow velocity is 142L/h, and dimethylbenzene is initially dense
Spend for 128ppm, air speed (GHSV) is 10000h-1。
3rd, absorption and catalytic treatment
At ambient temperature, mixture step 2 degraded is sent to the modified catalyst prepared equipped with step 1 with ozone
Hydrogen-catalyst reactor in, in the presence of cellular activated carbon, CO2、H2O and accessory substance are removed and mineralising；Wherein, catalyst
Consumption is 5.0g, and volume is about 12cm3, under normal temperature condition, the final dimethylbenzene obtained in product, ozone are detected,
Obtain testing result as shown in table 2.
Embodiment 3
1st, the preparation of modified catalyst
Commercially available cellular activated carbon is subjected to charing pretreatment at 600 DEG C, charing pre-treatment step is using conventional behaviour
Make technology, the mass fraction that then adulterates is modified for 3% manganese oxide, and doping process is to claim the cellular activated carbon after charing
Be impregnated into respectively after amount in the acetic acid manganese solution configured, impregnate 27h, after the completion of 11h is dried in 70 DEG C of air dry ovens, dry
After place into retort 400 DEG C of roasting temperatures under nitrogen atmosphere, under the high temperature conditions, acetic acid manganese solution is lived in honeycomb
Property carbon surface formation manganese oxide, obtain modified catalyst, wherein, the mass fraction of manganese oxide is 3%.
2nd, degradation treatment
Steam is passed into reaction of low temperature plasma device in advance, xylene waste gas is then passed into plasma again
Reactor, wherein, the volume ratio of steam and dimethylbenzene is 1:4, last dimethylbenzene is degraded into CO2、H2O and accessory substance etc. are mixed
Thing, also obtains harmful substance-ozone of low temperature plasma generation；Wherein, the applied voltage of plasma reactor is
16.9kV, the discharge power of plasma is 140.0w, and gas (i.e. xylene waste gas) flow velocity is 139L/h, and dimethylbenzene is initially dense
Spend for 131ppm, air speed (GHSV) is 10000h-1。
3rd, absorption and catalytic treatment
At ambient temperature, mixture step 2 degraded is sent to the modified catalyst prepared equipped with step 1 with ozone
Hydrogen-catalyst reactor in, CO2、H2O and accessory substance are removed；Wherein, catalyst amount is 6.2g, and volume is about 18cm3,
Under normal temperature condition, the final dimethylbenzene obtained in product, ozone are detected, testing result as shown in table 2 is obtained.
Embodiment 4
1st, the preparation of modified catalyst
Commercially available cellular activated carbon is subjected to charing pretreatment at 700 DEG C, charing pre-treatment step is using conventional behaviour
Make technology, the mass fraction that then adulterates is modified for 5% manganese oxide, and doping process is to claim the cellular activated carbon after charing
Be impregnated into respectively after amount in the acetic acid manganese solution configured, impregnate 22h, after the completion of 13h is dried in 90 DEG C of air dry ovens, dry
After place into retort 500 DEG C of roasting temperatures under nitrogen atmosphere, under the high temperature conditions, acetic acid manganese solution is lived in honeycomb
Property carbon surface formation manganese oxide, obtain modified catalyst, wherein, the mass fraction of manganese oxide is 5%.
2nd, degradation treatment
Steam is passed into reaction of low temperature plasma device in advance, xylene waste gas is then passed into plasma again
Reactor, wherein, the volumetric usage ratio of steam and xylene waste gas is 3：22, last dimethylbenzene is degraded into CO2、H2O and accessory substance
Deng mixture, harmful substance-ozone of low temperature plasma generation is also obtained；Wherein, the applied voltage of plasma reactor
For 17.6kV, the discharge power of plasma is 147.3w, and gas (i.e. xylene waste gas) flow velocity is 156L/h, and dimethylbenzene is initial
Concentration is 142ppm, and air speed (GHSV) is 10000h-1。
3rd, absorption and catalytic treatment
At ambient temperature, mixture step 2 degraded is sent to the modified catalyst prepared equipped with step 1 with ozone
Hydrogen-catalyst reactor in, in the presence of cellular activated carbon, CO2、H2O and accessory substance are removed and mineralising；Wherein, catalyst
Consumption is that 4.8g, volume is about 10cm3, under normal temperature condition, the final dimethylbenzene obtained in product, ozone are detected,
Obtain testing result as shown in table 2.
Embodiment 5
1st, the preparation of modified catalyst
Commercially available cellular activated carbon is subjected to charing pretreatment at 900 DEG C, charing pre-treatment step is using conventional behaviour
Make technology, the mass fraction that then adulterates is modified for 7% manganese oxide, and doping process is to claim the cellular activated carbon after charing
Be impregnated into respectively after amount in the acetic acid manganese solution configured, impregnate 24h, after the completion of 14h is dried in 100 DEG C of air dry ovens, dry
600 DEG C of roasting temperature 2.8h under nitrogen atmosphere are placed into retort after dry, under the high temperature conditions, acetic acid manganese solution exists
Cellular activated carbon surface forms manganese oxide, obtains modified catalyst, wherein, the mass fraction of manganese oxide is 7%.
2nd, degradation treatment
Steam is passed into reaction of low temperature plasma device in advance, xylene waste gas is then passed into plasma again
Reactor, wherein, the volumetric usage ratio of steam and xylene waste gas is 11：89, last dimethylbenzene is degraded into CO2、H2O and by-product
The mixtures such as thing, also obtain harmful substance-ozone of low temperature plasma generation；Wherein, the outer power-up of plasma reactor
Press as 17.6kV, the discharge power of plasma is 147.3w, at the beginning of gas (i.e. xylene waste gas) flow velocity is 156L/h, dimethylbenzene
Beginning concentration is 142ppm, and air speed (GHSV) is 10000h-1。
3rd, absorption and catalytic treatment
At ambient temperature, mixture step 2 degraded is sent to the modified catalyst prepared equipped with step 1 with ozone
Hydrogen-catalyst reactor in, wherein, catalyst amount is 5.4g, and volume is about 15cm3, under normal temperature condition, to final acquisition
Dimethylbenzene, ozone in product are detected, obtain testing result as shown in table 2.
Embodiment 6
1st, the preparation of modified catalyst
Commercially available cellular activated carbon is subjected to charing pretreatment at 800 DEG C, charing pre-treatment step is using conventional behaviour
Make technology, the mass fraction that then adulterates is modified for 2% manganese oxide, and doping process is to claim the cellular activated carbon after charing
Be impregnated into respectively after amount in the acetic acid manganese solution configured, impregnate 20h, after the completion of 14h is dried in 100 DEG C of air dry ovens, dry
500 DEG C of roasting temperature 2h under nitrogen atmosphere are placed into retort after dry, under the high temperature conditions, acetic acid manganese solution is in honeybee
Nest activated carbon surface formation manganese oxide, obtains modified catalyst, wherein, the mass fraction of manganese oxide is 2%.
2nd, degradation treatment
Steam is passed into reaction of low temperature plasma device in advance, xylene waste gas is then passed into plasma again
Reactor, wherein, the volumetric usage ratio of steam and xylene waste gas is 19：81, last dimethylbenzene is degraded into CO2、H2O and by-product
The mixtures such as thing, also obtain harmful substance-ozone of low temperature plasma generation；Wherein, the outer power-up of plasma reactor
Press as 17.6kV, the discharge power of plasma is 147.3w, at the beginning of gas (i.e. xylene waste gas) flow velocity is 156L/h, dimethylbenzene
Beginning concentration is 142ppm, and air speed (GHSV) is 10000h-1。
3rd, absorption and catalytic treatment
At ambient temperature, mixture step 2 degraded is sent to the modified catalyst prepared equipped with step 1 with ozone
Hydrogen-catalyst reactor in, wherein, catalyst amount is 5.3g, and volume is about 14cm3, under normal temperature condition, to final acquisition
Dimethylbenzene, ozone in product are detected, obtain testing result as shown in table 2.
Embodiment 7
1st, the preparation of modified catalyst
Commercially available cellular activated carbon is subjected to charing pretreatment at 700 DEG C, charing pre-treatment step is using conventional behaviour
Make technology, the mass fraction that then adulterates is modified for 4% manganese oxide, and doping process is to claim the cellular activated carbon after charing
Be impregnated into respectively after amount in the acetic acid manganese solution configured, impregnate 21h, after the completion of 13h is dried in 80 DEG C of air dry ovens, dry
After place into retort 600 DEG C of roasting temperature 2.8h under nitrogen atmosphere, under the high temperature conditions, acetic acid manganese solution is in honeybee
Nest activated carbon surface formation manganese oxide, obtains modified catalyst, wherein, the mass fraction of manganese oxide is 4%.
2nd, degradation treatment
Steam is passed into reaction of low temperature plasma device in advance, xylene waste gas is then passed into plasma again
Reactor, wherein, the volumetric usage ratio of steam and xylene waste gas is 21：79, last dimethylbenzene is degraded into CO2、H2O and by-product
The mixtures such as thing, also obtain harmful substance-ozone of low temperature plasma generation；Wherein, the outer power-up of plasma reactor
Press as 17.6kV, the discharge power of plasma is 147.3w, at the beginning of gas (i.e. xylene waste gas) flow velocity is 156L/h, dimethylbenzene
Beginning concentration is 142ppm, and air speed (GHSV) is 10000h-1。
3rd, absorption and catalytic treatment
At ambient temperature, mixture step 2 degraded is sent to the modified catalyst prepared equipped with step 1 with ozone
Hydrogen-catalyst reactor in, wherein, catalyst amount is 5.7g, and volume is about 16cm3, under normal temperature condition, to final acquisition
Dimethylbenzene, ozone in product are detected, obtain testing result as shown in table 2.
Embodiment 8
1st, the preparation of modified catalyst
Commercially available cellular activated carbon is subjected to charing pretreatment at 600 DEG C, charing pre-treatment step is using conventional behaviour
Make technology, the mass fraction that then adulterates is modified for 6% manganese oxide, and doping process is to claim the cellular activated carbon after charing
Be impregnated into respectively after amount in the acetic acid manganese solution configured, impregnate 24h, after the completion of 14h is dried in 90 DEG C of air dry ovens, dry
After place into retort 600 DEG C of roasting temperature 1.5h under nitrogen atmosphere, under the high temperature conditions, acetic acid manganese solution is in honeybee
Nest activated carbon surface formation manganese oxide, obtains modified catalyst, wherein, the mass fraction of manganese oxide is 6%.
2nd, degradation treatment
Steam is passed into reaction of low temperature plasma device in advance, xylene waste gas is then passed into plasma again
Reactor, wherein, the volumetric usage ratio of steam and xylene waste gas is 3：17, last dimethylbenzene is degraded into CO2、H2O and accessory substance
Deng mixture, harmful substance-ozone of low temperature plasma generation is also obtained；Wherein, the applied voltage of plasma reactor
For 17.6kV, the discharge power of plasma is 147.3w, and gas (i.e. xylene waste gas) flow velocity is 156L/h, and dimethylbenzene is initial
Concentration is 142ppm, and air speed (GHSV) is 10000h-1。
3rd, absorption and catalytic treatment
At ambient temperature, mixture step 2 degraded is sent to the modified catalyst prepared equipped with step 1 with ozone
Hydrogen-catalyst reactor in, wherein, catalyst amount is 5.8g, and volume is about 16cm3, under normal temperature condition, to final acquisition
Dimethylbenzene, ozone in product are detected, obtain testing result as shown in table 2.
The dimethylbenzene of table 2 and ozone removal efficiency testing result (%)
It can be seen from the testing result shown in table 2, the removal efficiency of the inventive method paraxylene can reach 100%, right
The removal efficiency of ozone reaches as high as 99%, it is seen then that the inventive method is good to VOCs removal effect.
A part of performance test of the tests below example for the present invention during research experiment, is only limitted to the explanation present invention's
Feature, not representing the research experiment of the present invention only includes tests below example.
Test example 1
This is applied to using the modified catalyst that acquisition is calcined under 300 DEG C, 400 DEG C, 500 DEG C, 600 DEG C of temperature conditionss
Inventive method paraxylene waste gas is handled, and is observed per 50min and is recorded the clearance of xylene waste gas, obtains such as Fig. 1 institutes
The removal efficiency design sketch shown.
It is according to Fig. 1 results, it can be seen that the inventive method not only removal efficiency is high, and persistence is strong, after 4h
Remain in that higher clearance.
As can be seen here, higher clearance can be achieved in the modified catalyst obtained under the conditions of above-mentioned sintering temperature.
Test example 2
Mass percent is used for the modified catalyst of 1%, 3%, 5%, 7% manganese oxide, applied to the inventive method pair
Xylene waste gas is handled, and is observed per 50min and is recorded the clearance of xylene waste gas, obtains removal efficiency as shown in Figure 2
Design sketch.
It is according to Fig. 2 results, it can be seen that the inventive method not only removal efficiency is high, and persistence is strong, after 4h
Remain in that higher clearance.
As can be seen here, manganese oxide mass percent content for 1%, 3%, 5%, 7% modified catalyst can be achieved compared with
High clearance.
Test example 3
The organic gas of dimethylbenzene will be purified using the inventive method purification dimethylbenzene organic gas and independent using plasma
Body carries out contrast test, compares the energy efficiency for removing dimethylbenzene, wherein, using plasma operating condition and embodiment
1 is identical.Obtain measurement result as shown in Figure 3.
Measurement result according to Fig. 3 can be seen that after addition activated carbon, and the energy efficiency of dimethylbenzene increases,
Energy efficiency increases with the reduction of energy density.When energy density is 10.26kJ/L, i.e., gas flow is 50L/h, single
The energy efficiency of only plasma technique is 2.13mg/kWh, and the energy efficiency of plasma body cooperative activated carbon technology is
2.78mg/kWh, improves 0.65mg/kWh.With the reduction of energy density, when energy density is 2.57kJ/L, i.e. gas stream
Measure as 200L/h, the energy efficiency of independent plasma technique is 8.18mg/kWh, the energy of plasma body cooperative activated carbon technology
Amount efficiency is 8.65mg/kWh.
The foregoing is only presently preferred embodiments of the present invention, be not intended to limit the invention, it is all the present invention spirit and
Any modifications, equivalent substitutions and improvements made within principle etc., should be included in the scope of the protection.
Claims (10)
1. a kind of method for the VOCs for removing low concentration big flow, it is characterised in that including：
Steam is passed into the internal reaction of low temperature plasma device provided with the metal electrode being fixed in dielectric in advance,
Make to produce in the reactor enough can react to form the free radical activity of stationary atom or molecule with other free radicals
Particle；
Volatile organic matter is passed through into the reactor for generating active particle, it is described to wave in the presence of high-tension current
Hair property organic matter is degraded, and is produced and is included CO2、H2O and accessory substance mixture；
The mixture is adsorbed and catalysis oxidation using modified catalyst, makes the ozone in the mixture is adsorbed to turn
Change, volatile organic matter is removed；
Wherein, the modified catalyst is by charing pretreatment and the modified cellular activated carbon of containing transition metal.
2. the method as described in claim 1, it is characterised in that the metal electrode is stainless steel bar, the dielectric is
Quartz glass, the reaction of low temperature plasma device is spool formula dielectric impedance reactor.
3. the method as described in claim 1, it is characterised in that the modified catalyst is to pre-process and adulterated by charing
Cross it is metal-modified after cellular activated carbon.
4. method as claimed in claim 4, it is characterised in that mass percent of the transition metal in modified activated carbon
For 1-7%.
5. method as claimed in claim 3, it is characterised in that the transition metal is Mn.
6. a kind of modified catalyst for being used to remove VOCs, it is characterised in that it is the transition gold that pre-processes and adulterate by charing
The modified cellular activated carbon of category, is prepared by following steps：
Cellular activated carbon is subjected to charing pretreatment under nitrogen atmosphere；
Pretreated cellular activated carbon will be carbonized and be immersed in acetic acid manganese solution, acetic acid manganese solution is fully penetrated into honeycomb activity
In charcoal；
The cellular activated carbon for being impregnated with acetic acid manganese solution is dried after processing, dried cellular activated carbon is obtained；
The cellular activated carbon of the acquisition is subjected to calcination process in nitrogen atmosphere, modified catalyst is obtained.
7. modified catalyst as claimed in claim 6, it is characterised in that the temperature of the charing pretreatment is 500 DEG C -900
℃。
8. modified catalyst as claimed in claim 6, it is characterised in that the drying process temperature is 60-100 DEG C, drying
Shi Changwei 10-14h.
9. modified catalyst as claimed in claim 6, it is characterised in that the calcination process temperature is 300-600 DEG C, roasting
Duration 1.5-3.5h.
10. a kind of modified catalyst by described in claim 6 is used for produced by after reaction of low temperature plasma device degraded VOCs
Include the accessory substance of ozone.
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Application publication date: 20171107 |