CN108325379A - A kind of method and its dedicated unit using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning - Google Patents
A kind of method and its dedicated unit using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning Download PDFInfo
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- CN108325379A CN108325379A CN201810087733.1A CN201810087733A CN108325379A CN 108325379 A CN108325379 A CN 108325379A CN 201810087733 A CN201810087733 A CN 201810087733A CN 108325379 A CN108325379 A CN 108325379A
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- spinel structure
- flue gas
- based spinel
- magnetic iron
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- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 137
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 73
- 239000003546 flue gas Substances 0.000 title claims abstract description 73
- 229910052742 iron Inorganic materials 0.000 title claims abstract description 63
- 239000000463 material Substances 0.000 title claims abstract description 58
- 239000012855 volatile organic compound Substances 0.000 title claims abstract description 57
- 229910052596 spinel Inorganic materials 0.000 title claims abstract description 56
- 239000011029 spinel Substances 0.000 title claims abstract description 56
- 238000000034 method Methods 0.000 title claims abstract description 49
- 238000000746 purification Methods 0.000 title claims abstract description 17
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims abstract description 45
- 239000007788 liquid Substances 0.000 claims abstract description 34
- 229910052751 metal Inorganic materials 0.000 claims abstract description 6
- 239000002184 metal Substances 0.000 claims abstract description 6
- 238000006243 chemical reaction Methods 0.000 claims description 71
- 239000007789 gas Substances 0.000 claims description 45
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 claims description 15
- SZVJSHCCFOBDDC-UHFFFAOYSA-N iron(II,III) oxide Inorganic materials O=[Fe]O[Fe]O[Fe]=O SZVJSHCCFOBDDC-UHFFFAOYSA-N 0.000 claims description 10
- 230000005389 magnetism Effects 0.000 claims description 9
- 150000001298 alcohols Chemical class 0.000 claims description 3
- 150000001299 aldehydes Chemical class 0.000 claims description 3
- 238000000975 co-precipitation Methods 0.000 claims description 3
- 229910052802 copper Inorganic materials 0.000 claims description 3
- 150000002148 esters Chemical class 0.000 claims description 3
- 150000002170 ethers Chemical class 0.000 claims description 3
- 150000002576 ketones Chemical class 0.000 claims description 3
- 229910052748 manganese Inorganic materials 0.000 claims description 3
- 238000011084 recovery Methods 0.000 claims description 3
- 229910052719 titanium Inorganic materials 0.000 claims description 3
- 230000001052 transient effect Effects 0.000 claims description 3
- 239000002699 waste material Substances 0.000 claims description 3
- 229910052725 zinc Inorganic materials 0.000 claims description 3
- 230000008569 process Effects 0.000 abstract description 8
- 230000000694 effects Effects 0.000 abstract description 6
- 230000015556 catabolic process Effects 0.000 abstract description 5
- 238000006731 degradation reaction Methods 0.000 abstract description 5
- 238000005516 engineering process Methods 0.000 abstract description 5
- 238000010438 heat treatment Methods 0.000 abstract description 4
- 230000004308 accommodation Effects 0.000 abstract description 3
- 239000002253 acid Substances 0.000 abstract description 3
- 239000002585 base Substances 0.000 abstract description 3
- 239000010802 sludge Substances 0.000 abstract description 3
- 239000003513 alkali Substances 0.000 abstract description 2
- 230000007797 corrosion Effects 0.000 abstract description 2
- 238000005260 corrosion Methods 0.000 abstract description 2
- 239000000243 solution Substances 0.000 description 34
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 15
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 14
- YMWUJEATGCHHMB-UHFFFAOYSA-N Dichloromethane Chemical compound ClCCl YMWUJEATGCHHMB-UHFFFAOYSA-N 0.000 description 12
- 238000010521 absorption reaction Methods 0.000 description 12
- 239000003054 catalyst Substances 0.000 description 12
- IKHGUXGNUITLKF-UHFFFAOYSA-N Acetaldehyde Chemical compound CC=O IKHGUXGNUITLKF-UHFFFAOYSA-N 0.000 description 11
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 11
- 238000007254 oxidation reaction Methods 0.000 description 11
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 description 10
- 229910002092 carbon dioxide Inorganic materials 0.000 description 9
- 239000003344 environmental pollutant Substances 0.000 description 9
- 231100000719 pollutant Toxicity 0.000 description 9
- 238000002360 preparation method Methods 0.000 description 9
- 230000009102 absorption Effects 0.000 description 8
- -1 hydroxyl radical free radical Chemical class 0.000 description 8
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 7
- 230000003647 oxidation Effects 0.000 description 7
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 6
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 description 5
- 239000001569 carbon dioxide Substances 0.000 description 5
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 4
- 239000007791 liquid phase Substances 0.000 description 4
- 239000000047 product Substances 0.000 description 4
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 229910001882 dioxygen Inorganic materials 0.000 description 3
- 238000007210 heterogeneous catalysis Methods 0.000 description 3
- 230000007246 mechanism Effects 0.000 description 3
- 229910021645 metal ion Inorganic materials 0.000 description 3
- 238000000465 moulding Methods 0.000 description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 3
- 239000005416 organic matter Substances 0.000 description 3
- 239000007800 oxidant agent Substances 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 229910000831 Steel Inorganic materials 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- NEHMKBQYUWJMIP-UHFFFAOYSA-N chloromethane Chemical class ClC NEHMKBQYUWJMIP-UHFFFAOYSA-N 0.000 description 2
- 238000010276 construction Methods 0.000 description 2
- 230000005611 electricity Effects 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000012071 phase Substances 0.000 description 2
- 238000012545 processing Methods 0.000 description 2
- 238000003672 processing method Methods 0.000 description 2
- 239000007921 spray Substances 0.000 description 2
- 239000010959 steel Substances 0.000 description 2
- 231100000331 toxic Toxicity 0.000 description 2
- 230000002588 toxic effect Effects 0.000 description 2
- 238000004056 waste incineration Methods 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 1
- 208000005623 Carcinogenesis Diseases 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 description 1
- CKUAXEQHGKSLHN-UHFFFAOYSA-N [C].[N] Chemical compound [C].[N] CKUAXEQHGKSLHN-UHFFFAOYSA-N 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 238000013475 authorization Methods 0.000 description 1
- 230000005587 bubbling Effects 0.000 description 1
- 230000036952 cancer formation Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 231100000504 carcinogenesis Toxicity 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 125000003963 dichloro group Chemical group Cl* 0.000 description 1
- 239000010791 domestic waste Substances 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000003628 erosive effect Effects 0.000 description 1
- DNJIEGIFACGWOD-UHFFFAOYSA-N ethanethiol Chemical compound CCS DNJIEGIFACGWOD-UHFFFAOYSA-N 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 229910001448 ferrous ion Inorganic materials 0.000 description 1
- 239000011790 ferrous sulphate Substances 0.000 description 1
- 235000003891 ferrous sulphate Nutrition 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 239000012467 final product Substances 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 description 1
- RUTXIHLAWFEWGM-UHFFFAOYSA-H iron(3+) sulfate Chemical compound [Fe+3].[Fe+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O RUTXIHLAWFEWGM-UHFFFAOYSA-H 0.000 description 1
- 229910000359 iron(II) sulfate Inorganic materials 0.000 description 1
- 229910000360 iron(III) sulfate Inorganic materials 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 238000003032 molecular docking Methods 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 238000005325 percolation Methods 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 150000003254 radicals Chemical class 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 150000003384 small molecules Chemical class 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 239000002912 waste gas Substances 0.000 description 1
Classifications
-
- 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
-
- 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
- B01J23/70—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
- B01J23/78—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 alkali- or alkaline earth metals
-
- B01J35/33—
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/10—Oxidants
- B01D2251/106—Peroxides
-
- 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
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2258/00—Sources of waste gases
- B01D2258/02—Other waste gases
- B01D2258/0283—Flue gases
- B01D2258/0291—Flue gases from waste incineration plants
Abstract
The invention discloses a kind of methods and its dedicated unit using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning, this method is arranged using solid-liquid two-phase using magnetic iron-based spinel structure material and the hydrogen peroxide solution of humble concentration, flue gas of refuse burning is wherein passed through from solid-liquid system, you can remove VOCs therein.Compared with the existing technology, the present invention provides a kind of new methods based on VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning, this method can avoid a large amount of electric energy that iron sludge pollution and heating means consume, without additional addition acid-base accommodation, avoid generating acid and alkali corrosion effect to metal equipment surface, it is simple for process in addition, it is at low cost, the degradation efficiency of VOCs is high, is a kind of efficient, environmentally friendly, cheap method, easy to utilize.
Description
Technical field
The invention discloses a kind of sides using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning
Method and its dedicated unit belong to flue gas pollutant control technology field.
Background technology
With the increasingly raising of life of urban resident level, the processing of domestic waste more uses waste incineration electricity
The mode of factory.However, the volatile organism VOCs of flue gas of refuse burning discharge has obtained both at home and abroad the harm of natural environment
Further concern.VOCs gases include mainly a series of organic compounds such as aldehydes, alcohols, benzene homologues, esters, ethers, ketone
Object.VOCs, which sucks human body, has strong carcinogenesis.
Processing to VOCs pollutants in flue gas of refuse burning is always research focus both domestic and external.Currently used rubbish
VOCs processing methods mainly have physisorphtion (such as activated carbon adsorption), heat treating process (such as high temperature burn point again in incineration flue gas
Solution) and chemical absorption method (such as oxidizing agent solution absorption).The VOCs that physisorphtion is handled in flue gas of refuse burning can only be simple
It by contaminant transportation, cannot thoroughly be degraded, the VOCs after absorption has the risk of secondary volatilization；Heat treating process is efficiently rapid,
VOCs can be effectively degraded to carbon dioxide, but this method needs higher ignition temperature, consumes a large amount of heat.Chemical treatment
Technology can be comparatively fast by VOCs oxidations, the degradation in flue gas of refuse burning, but traditional homogeneous oxidizing agent is expensive, uses one
The problems such as being not easy to recycle, easily cause secondarily polluted water after the section time, selects proper heterogeneous phase chemistry oxidant can be by rubbish
VOCs in rubbish incineration flue gas is degraded to carbon dioxide, does not generate secondary pollution.
A kind of flue gas of refuse burning is disclosed in Chinese invention patent (102698578 A of Publication No. CN) application documents
The method of middle nitrogen oxides, bioxin and stench, it is by using reproducibility catalyst and sprays ammonia means by the pollution in flue gas
Object selective reduction is at nitrogen and carbon dioxide.It is public in Chinese invention patent (106621744 A of Publication No. CN) application documents
A kind of VOCs waste gas processing methods are opened, this method flows through the electronics with high-energy using hydrogen peroxide steam and vapor and fills
In setting so that hydrogen peroxide steam and vapor ionization are decomposed and generated free radicals, to aoxidize the VOCs in flue gas.This method has
Have and aoxidize efficient, the fireballing advantage of organic matter degradation, but high energy electron needs electron irradiation pipe to generate, invests operating cost
It is higher.In general, the VOCs pollutants in flue gas of refuse burning have the characteristics that big toxicity, high volatility, removing difficulty are high.
Chinese patent (Authorization Notice No. be 206325367 U of CN) discloses a kind of VOCs tail gas absorptions purifier, but simply by
Bubbling device simply washs the flue gas containing VOCs, to oxide-reduction method in device without reference to.
Invention content
Goal of the invention：In view of the above technical problems, magnetic iron-based spinel structure material is utilized the present invention provides a kind of
The method and its dedicated unit of VOCs in purifying flue gas of refuse burning, this method has efficiently quickly, of low cost, environment friend
Well, the VOCs in flue gas of refuse burning, can be degraded to by the advantages of not generating secondary pollution by Heterogeneous oxidation means
Carbon dioxide solves the problems, such as that the prior art is low to the VOCs removal efficiencies in flue gas of refuse burning.
Technical solution：The present invention provides a kind of using in magnetic iron-based spinel structure materials purification flue gas of refuse burning
The method of VOCs, magnetic iron-based spinel structure material and the hydrogen peroxide solution of humble concentration are arranged using solid-liquid two-phase, by rubbish
Rubbish incineration flue gas wherein passes through from solid-liquid system, you can removes VOCs therein；
The magnetism iron-based spinel structure material is Fe3O4Or its transient metal doped derivative Fe3-xMxO4, wherein
M be Ti, Mn, Cu, Zn one or two, 0<x<1；The hydrogen peroxide solution of the humble concentration, a concentration of 0.001~
0.5mol/L。
The magnetism iron-based spinel structure material is porous structure, and specific surface area is 200~500m2/ g can make
With after a period of time by be separated by solid-liquid separation, recycled by regeneration means.
The pH value of the hydrogen peroxide solution is 6.0~8.0.
The mass ratio of the magnetism iron-based spinel structure material and hydrogen peroxide solution is 1:50~1:1000.
The magnetism iron-based spinel structure material is prepared using coprecipitation, and stable in physicochemical property, metal ion filters out
Rate is low, non-secondary pollution, Fe3-xMxO4Ranging from the 0 of middle x<x<0.8.
Temperature when the VOCs removings is controlled at 100~200 DEG C.
The VOCs is toxic and volatile organic pollution, including but not limited to aldehydes, alcohols, benzene homologues, esters, ether
Class, ketone etc..
The present invention also provides the dedicated units of the above method, including reaction tower body, gas inlet, exhanst gas outlet, placement
Mesh-supported frame, the reaction gentle body distributor of nozzle for liquid, gas inlet and the exhanst gas outlet of magnetic iron-based spinel structure material
It is respectively arranged on bottom sidewall and the top of reaction tower body, inside reaction tower body, between gas inlet and exhanst gas outlet, is set successively
Set gas distributor, mesh-supported frame and reaction nozzle for liquid, the hydrogen peroxide solution supply arrangement outside reaction nozzle for liquid connection.
The hydrogen peroxide solution supply arrangement includes dioxygen water store tank and coupled first circulation pump and second
Circulating pump, first circulation pump other end connection reaction tower body bottom sidewall, and second circulation pumps other end connection reaction nozzle for liquid.
Further, which further includes the third circulating pump of connection reaction tower body bottom, the third circulating pump other end
Connect waste recovery area.
The application method of the dedicated unit is：
Above-mentioned oxidation reaction system is placed in absorbing reaction tower, flue gas self-absorption tower bottom introduces, and passes through absorption tower bottom
The gas distributor in portion is dispersed into uniform air flow and enters reaction system liquid phase region, flows up through magnetic iron-based spinel structure material
(magnetic iron-based spinel structure material is placed in molding mesh-supported steel frame construction, and reticular supporting structure is placed in hydrogen peroxide afterwards
In solution), liquid phase region is flowed out, absorption tower is discharged in self-absorption top of tower.
When reaction, hydrogen peroxide solution is normal temperature and pressure, and gas liquid ratio is 6~28L/m in reaction tower3, temperature control 100~
200℃。
The present invention forms heterogeneous height using the magnetism iron-based spinel structure material and the hydrogen peroxide solution of humble concentration
Grade oxidation reaction system, by following two-step methods by VOCs oxidation removals in flue gas of refuse burning：
The first step, for magnetic iron-based spinel structure material as solid-liquid heterogeneous catalysis, the dioxygen of humble concentration is water-soluble
Liquid is mixed in a certain ratio with magnetic iron-based spinel structure material, and the oxidation with magnetic iron-based spinel structure material surface is also
First wife's docking, which touches to decompose, generates the hydroxyl radical free radical of strong oxidation.Magnetic iron-based spinel structure material physicochemical property is steady
It is fixed, it derives from a wealth of sources, metal ion percolation rate is low, does not generate secondary pollution.
The mechanism that wherein hydroxyl radical free radical is generated in magnetic iron-based spinel structure material surface is：
≡Fe2++H2O2→≡Fe3++·OH+OH-
≡Fe3++H2O2→≡Fe3+H2O2
≡Fe3+H2O2→≡Fe2++·HO2+H+
≡Fe3++·HO2→≡Fe2++O2+H+
≡Mn++H2O2→≡M(n+1)++·OH+OH-
≡M(n+1)++H2O2→≡M(n+1)+H2O2
≡M(n+1)+H2O2→≡Mn++·HO2+H+
≡M(n+1)++·HO2→≡Mn++O2+H+
≡M(n+1)++≡Fe2+→≡Fe3++≡Mn+
Second step, when the flue gas of refuse burning containing VOCs pollutants flows into above-mentioned reaction system, hydroxyl radical free radical passes through
Effect of mass transmitting rapidly enters gas-liquid surface, is small soluble molecules organic matter by organic pollution initial oxidation, then can by small molecule
Molten organic matter continues to aoxidize, until being all degraded to carbon dioxide.Experiment shows reachable lower hydrogen peroxide concentration
To higher reactivity, final product is nuisanceless product, environmentally friendly.
Wherein hydroxyl radical free radical is with VOCs pollutant reactions mechanism in flue gas：
CH2O+·OH→CO2+H2O
CH3CHO+·OH→CO2+H2O
C6H6+·OH→CO2+H2O
C7H8+·OH→CO2+H2O
CΗ3Cl+·ΟΗ→CΟ2+Η2Ο+HCl
New method provided by the invention based on VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning,
Catalytic mechanism when the magnetic iron-based spinel structure material that this method uses is as catalyst is heterogeneous catalysis, without addition
Iron ion is not necessarily to heating means, so that it may which the hydrogen peroxide to be catalyzed humble concentration generates a large amount of hydroxyl radical free radical, can both efficiently
Various pollutants molecule in flue gas of refuse burning is quickly attacked again, so that it is lost and is electronically formed high oxide, avoids molten
A large amount of electric energy of iron sludge pollution and heating means consumption that a large amount of iron ions are brought are added in liquid.
The method of the present invention also utilizes the hydrogen peroxide solution of the humble concentration of normal temperature and pressure, is applicable in the pH of solution in neutral conditions
Higher oxidation effectiveness is can reach, there is no need to additionally add acid-base accommodation, avoids generating soda acid corruption to metal equipment surface
Erosion acts on.
New method provided by the invention based on VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning,
The back-end ductwork of burning power plant is may be arranged at, the optimum temperature of the oxidation reaction is controlled at 100~200 DEG C, at this
In temperature range, this method can be used in combination with existing pollutant process equipment, such as be placed in the downstream of dust catcher device,
Alternative existing denitration device and VOCs cleaning equipments.
The new method provided through the invention, the degradation efficiency of VOCs can reach 96% or more in flue gas of refuse burning,
It realizes that multiple pollutant removes simultaneously in a reaction unit, reaches the discharge of VOCs in the flue gas of refuse burning of national regulation
Standard.
Technique effect：Compared with the existing technology, it is net based on magnetic iron-based spinel structure material that the present invention provides one kind
Change the new method of VOCs in flue gas of refuse burning, this method can avoid a large amount of electricity that iron sludge pollution and heating means consume
Can, without additional addition acid-base accommodation, avoid generating acid and alkali corrosion effect to metal equipment surface, it is simple for process in addition, at
This is low, and the degradation efficiency of VOCs is high, is a kind of efficient, environmentally friendly, cheap method, easy to utilize.
Description of the drawings
Fig. 1 is dedicated unit of the present invention using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning
Structural schematic diagram, wherein 2 be reaction solution in tower.
Specific implementation mode
The specific implementation mode of VOCs methods is in purifying flue gas of refuse burning provided by the invention：
Dedicated unit is：
As shown in Figure 1, including reaction tower body 1, gas inlet 1-1, exhanst gas outlet 1-2, placing magnetic iron-based spinelle knot
The mesh-supported frame 3 of structure material, reaction nozzle for liquid 4 and gas distributor 6, gas inlet 1-1 and exhanst gas outlet 1-2 are respectively arranged on
Bottom sidewall and the top for reacting tower body 1, react inside tower body 1, between gas inlet 1-1 and exhanst gas outlet 1-2, set successively
Gas distributor 6, mesh-supported frame 3 and reaction nozzle for liquid 4 are set, reaction nozzle for liquid 4 connects external hydrogen peroxide solution supply and sets
It is standby.
Hydrogen peroxide solution supply arrangement includes that dioxygen water store tank 5 and coupled first circulation pump 7 and second follow
Ring pump 9, first circulation pump 7 other ends connection reaction 1 bottom sidewall of tower body, and second circulation pumps 9 other ends connection reaction nozzle for liquid
4。
The dedicated unit further includes the third circulating pump 8 of 1 bottom of connection reaction tower body, the connection of 8 other end of third circulating pump
Waste recovery area 10.
The application method of the dedicated unit is：
Above-mentioned oxidation reaction system is placed in absorbing reaction tower, flue gas self-absorption tower bottom introduces, and passes through absorption tower bottom
The gas distributor in portion is dispersed into uniform air flow and enters reaction system liquid phase region, flows up through magnetic iron-based spinel structure material
(magnetic iron-based spinel structure material is placed in molding mesh-supported steel frame construction, and reticular supporting structure is placed in hydrogen peroxide afterwards
In solution), liquid phase region is flowed out, absorption tower is discharged in self-absorption top of tower.
When reaction, hydrogen peroxide solution is normal temperature and pressure, and gas liquid ratio is 6~28L/m in reaction tower3, temperature control 100~
200℃。
The present invention is based on the new method of VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning is as follows：
(1) the magnetic iron-based spinel structure material Fe of different metal ions doping ratio is prepared by coprecipitation3O4And
Its transient metal doped derivative Fe3-xMxO4, M Ti, Mn, Cu, Zn one or two, wherein 0<x<1.Preparation method is：
The ferrous sulfate of the ferric sulfate, 0.3-0.5mol/L that configure 0.5-0.7mol/L (ensures the molar ratio of iron ion and ferrous ion
It is 3:And the quasi- chloride MCl for wanting containing transition metal of 0.03-0.6mol/L 2)n, then gradually instill the hydrogen of 3-4mol/L
In sodium hydroxide solution, in the process, keeps 65 DEG C of constant temperature of mixed solution and be stirred with the speed of 600-800r/min, dripped
Porous molecular screen carrier is added while adding, the wherein mass ratio of carrier and heterogeneous catalysis is (5-10):1.It mixes after the completion
Close product constant temperature and stand 2h, after dark green to be generated precipitation becomes black particle completely, wash away particle surface it is soluble from
Son, filtration drying molding.Ensure the active component stable structure of magnetic iron-based spinel structure material surface, loss is less, makes
With not generating the substance done harm to environmental toxic in the process.
(2) the magnetic iron-based spinel structure material prepared is made to the particle of diameter 10mm or so, ensures that air-flow is suitable
Profit passes through, and is then divided into variety classes and ratio, is added in the catalyst supporting structure of reaction tower (mesh-supported frame 3), will
The hydrogen peroxide solution of humble concentration is added to above-mentioned reaction tower, it is made not have catalyst supporting structure.The addition of hydrogen peroxide solution
The pH value of a concentration of 0.001~0.5mol/L, hydrogen peroxide solution are 6.0~8.0, hydrogen peroxide solution and iron-based spinel structure material
Material in mass ratio 50:1~1000:1 adds.
(3) it is directed to the flue gas of refuse burning containing various concentration and pollutant species, superficial linear velocity in a column is controlled in 5000-
50000h-1。
(4) after reaction starts, the change that VOCs concentration becomes in reaction solution and flue gas, overall merit waste incineration are detected respectively
The removal effect of VOCs in flue gas；After reaction, by detecting respectively in solution and magnetic iron-based spinel structure material
The carbon nitrogen regularity of distribution, the clean-up effect of VOCs in overall merit flue gas of refuse burning.
In order to make the purpose of the present invention and technical solution be more clearly understood, following embodiment does further in detail the present invention
It describes in detail bright.It should be appreciated that described herein, specific examples are only used to explain the present invention, is not intended to limit the present invention.This
Outside, technical characteristic involved in each embodiment of invention described below as long as they do not conflict with each other can
To be combined with each other.
Embodiment 1：
Modulus intends the flue gas of burning power plant, and flue-gas temperature is 125 DEG C, a concentration of 15g/m of acetaldehyde in flue gas3.
The magnetic iron-based spinel structure material Fe of preparation is added in reaction tower catalyst support device3O4, specific surface area 215m2/
g.The H of 0.5mol/L concentration is prepared under room temperature2O2Solution, pH 6.4, H2O2Solution and Fe3O4Mass ratio is 1000:1, uniformly spray
It spills into above-mentioned reaction system, gas liquid ratio is 6L/m in reaction tower3, superficial linear velocity in a column control is in 5000h-1.It is detected respectively after 30min
The acetaldehyde concentration variation of reaction solution, exhanst gas outlet.
The removal efficiency of acetaldehyde is 96%.
Embodiment 2：
Modulus intends the flue gas of burning power plant, and flue-gas temperature is 105 DEG C, a concentration of 9.5g/m of toluene in flue gas3.
The magnetic iron-based spinel structure material Fe of preparation is added in reaction tower catalyst support device2.6Mn0.4O4, specific surface area is
298m2/g.The H of 0.03mol/L concentration is prepared under room temperature2O2Solution, pH 6.8, H2O2Solution and Fe3O4Mass ratio is 800:1,
It is uniformly sprayed in above-mentioned reaction system, gas liquid ratio is 12L/m in reaction tower3, superficial linear velocity in a column control is in 7000h-1.After 30min
The toluene concentration variation of reaction solution, exhanst gas outlet is detected respectively.
The removal efficiency of toluene is 98%.
Embodiment 3：
Modulus intends the flue gas of burning power plant, and flue-gas temperature is 165 DEG C, a concentration of 18g/ of dichloromethane in flue gas
m3.The magnetic iron-based spinel structure material Fe of preparation is added in reaction tower catalyst support device2.7Ti0.3O4, specific surface
Product is 252m2/g.The H of 0.01mol/L concentration is prepared under room temperature2O2Solution, pH 6.8, H2O2Solution and Fe3O4Mass ratio is
500:1, it is uniformly sprayed in above-mentioned reaction system, gas liquid ratio is 28L/m in reaction tower3, superficial linear velocity in a column control is in 30000h-1。
The concentration dichloromethane variation of reaction solution, exhanst gas outlet is detected after 30min respectively.
The removal efficiency of dichloromethane is 98%.
Embodiment 4：
Modulus intends the flue gas of burning power plant, and flue-gas temperature is 195 DEG C, a concentration of 30g/m of acetone in flue gas3.
The magnetic iron-based spinel structure material Fe of preparation is added in reaction tower catalyst support device2.7Cu0.3O4, specific surface area is
437m2/g.The H of 0.008mol/L concentration is prepared under room temperature2O2Solution, pH 7.2, H2O2Solution and Fe3O4Mass ratio is 200:
1, it is uniformly sprayed in above-mentioned reaction system, gas liquid ratio is 18L/m in reaction tower3, superficial linear velocity in a column control is in 20000h-1。30min
Detect the acetone concentration variation of reaction solution, exhanst gas outlet respectively afterwards.
The removal efficiency of acetone is 96%.
Embodiment 5：
Modulus intends the flue gas of burning power plant, and flue-gas temperature is 170 DEG C, a concentration of 5g/m of isopropanol in flue gas3.
The magnetic iron-based spinel structure material Fe of preparation is added in reaction tower catalyst support device2.7Zn0.3O4, specific surface area is
326m2/g.The H of 0.09mol/L concentration is prepared under room temperature2O2Solution, pH 6.7, H2O2Solution and Fe3O4Mass ratio is 600:1,
It is uniformly sprayed in above-mentioned reaction system, gas liquid ratio is 24L/m in reaction tower3, superficial linear velocity in a column control is in 10000h-1.After 30min
The isopropyl alcohol concentration variation of reaction solution, exhanst gas outlet is detected respectively.
The removal efficiency of isopropanol is 97%.
Embodiment 6：
Modulus intends the flue gas of burning power plant, and flue-gas temperature is 110 DEG C, a concentration of 7g/m of styrene in flue gas3.
The magnetic iron-based spinel structure material Fe of preparation is added in reaction tower catalyst support device2.7Cu0.2Zn0.1O4, specific surface
Product is 496m2/g.The H of 0.001mol/L concentration is prepared under room temperature2O2Solution, pH 7.8, H2O2Solution and Fe3O4Mass ratio is
50:1, it is uniformly sprayed in above-mentioned reaction system, gas liquid ratio is 20L/m in reaction tower3, superficial linear velocity in a column control is in 20000h-1。
The concentration of styrene variation of reaction solution, exhanst gas outlet is detected after 30min respectively.
The removal efficiency of styrene is 99%.
Embodiment 7：
Modulus intends the flue gas of burning power plant, and flue-gas temperature is 196 DEG C, a concentration of 6g/m of toluene in flue gas3, dichloro
A concentration of 12g/m of methane3, a concentration of 5g/m of isopropanol3, a concentration of 7g/m of styrene3.In reaction tower catalyst support
The magnetic iron-based spinel structure material Fe of preparation is added in device2.7Cu0.2Zn0.1O4, specific surface area 496m2/g.Room temperature
The lower H for preparing 0.01mol/L concentration2O2Solution, pH 6.7, H2O2Solution and Fe3O4Mass ratio is 300:1, uniformly it is sprayed to
It states in reaction system, gas liquid ratio is 16L/m in reaction tower3, superficial linear velocity in a column control is in 50000h-1.Detection reaction respectively after 30min
The VOCs concentration variation of liquid, exhanst gas outlet.
The removal efficiency of toluene is 97%, and the removal efficiency of dichloromethane is 96%, and the removal efficiency of isopropanol is 96%, styrene
Removal efficiency be 98%.
Embodiment 8：
Modulus intends the flue gas of burning power plant, and flue-gas temperature is 183 DEG C, a concentration of 16g/m of acetaldehyde in flue gas3, benzene
A concentration of 9g/m3, a concentration of 4g/m of dimethylbenzene3, a concentration of 15g/m of formaldehyde3, a concentration of 17g/m of chloromethanes3.Anti-
Answer the magnetic iron-based spinel structure material Fe that preparation is added in tower catalyst support device2.6Cu0.2Mn0.2O4, specific surface area
For 427m2/g.The H of 0.06mol/L concentration is prepared under room temperature2O2Solution, pH 6.4, H2O2Solution and Fe3O4Mass ratio is 400:
1, it is uniformly sprayed in above-mentioned reaction system, gas liquid ratio is 16L/m in reaction tower3, superficial linear velocity in a column control is in 40000h-1。30min
Detect the VOCs concentration variation of reaction solution, exhanst gas outlet respectively afterwards.
The removal efficiency of acetaldehyde is 96%, and the removal efficiency of benzene is 95%, and the removal efficiency of dimethylbenzene is 99%, the removal efficiency of formaldehyde
It is 99%, the removal efficiency of chloromethanes is 98%.
The present invention can be described with others without prejudice to the concrete form of the spirit or essential characteristics of the present invention.The present invention's
The embodiment above is only the preferred embodiment in implementation process of the present invention, can only be considered the explanation of the present invention rather than limit
It makes, any trickle amendment made by every substantial technological according to the present invention and same replacement, in protection scope of the present invention
Within.
Claims (10)
1. a kind of method using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning, which is characterized in that
The hydrogen peroxide solution of magnetic iron-based spinel structure material and humble concentration using solid-liquid two-phase arrangement, by flue gas of refuse burning from
Solid-liquid system wherein passes through, you can removes VOCs therein；
The magnetism iron-based spinel structure material is Fe3O4Or its transient metal doped derivative Fe3-xMxO4, wherein M is
The one or two of Ti, Mn, Cu, Zn, 0<x<1；The hydrogen peroxide solution of the humble concentration, a concentration of 0.001~0.5mol/
L。
2. the side according to claim 1 using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning
Method, which is characterized in that the magnetism iron-based spinel structure material is porous structure, and specific surface area is 200~500m2/g。
3. the side according to claim 1 using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning
Method, which is characterized in that the pH value of the hydrogen peroxide solution is 6.0~8.0.
4. the side according to claim 1 using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning
Method, which is characterized in that the mass ratio of the magnetism iron-based spinel structure material and hydrogen peroxide solution is 1:50~1:1000.
5. the side according to claim 1 using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning
Method, which is characterized in that the magnetism iron-based spinel structure material is prepared using coprecipitation, Fe3-xMxO4Ranging from the 0 of middle x<
x<0.8。
6. the side according to claim 1 using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning
Method, which is characterized in that the temperature when VOCs removings is controlled at 100~200 DEG C.
7. the side according to claim 1 using VOCs in magnetic iron-based spinel structure materials purification flue gas of refuse burning
Method, the VOCs are aldehydes, alcohols, benzene homologues, esters, ethers or ketone.
8. the dedicated unit of any one of claim 1-7 the methods, which is characterized in that including reaction tower body (1), gas inlet
(1-1), exhanst gas outlet (1-2), the mesh-supported frame (3) for placing magnetic iron-based spinel structure material, reaction nozzle for liquid (4) and
Gas distributor (6), gas inlet (1-1) and exhanst gas outlet (1-2) are respectively arranged on bottom sidewall and the top of reaction tower body (1)
Portion, reaction tower body (1) is internal, between gas inlet (1-1) and exhanst gas outlet (1-2), set gradually gas distributor (6),
Mesh-supported frame (3) and reaction nozzle for liquid (4) react the hydrogen peroxide solution supply arrangement outside nozzle for liquid (4) connection.
9. dedicated unit according to claim 8, which is characterized in that the hydrogen peroxide solution supply arrangement includes hydrogen peroxide
Holding vessel (5) and coupled first circulation pump (7) and second circulation pump (9), it is anti-that first circulation pumps the connection of (7) other end
Tower body (1) bottom sidewall, second circulation is answered to pump (9) other end connection reaction nozzle for liquid (4).
10. dedicated unit according to claim 8, which is characterized in that further include the third of connection reaction tower body (1) bottom
Circulating pump (8), third circulating pump (8) other end connect waste recovery area (10).
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Application publication date: 20180727 |