CN116371193A - Hydroxyl metal oxide catalyst, preparation method and application thereof in plasma synergistic catalysis waste gas treatment - Google Patents
Hydroxyl metal oxide catalyst, preparation method and application thereof in plasma synergistic catalysis waste gas treatment Download PDFInfo
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- 239000003054 catalyst Substances 0.000 title claims abstract description 39
- 229910044991 metal oxide Inorganic materials 0.000 title claims abstract description 35
- -1 Hydroxyl metal oxide Chemical class 0.000 title claims abstract description 34
- 238000002360 preparation method Methods 0.000 title claims abstract description 12
- 239000002912 waste gas Substances 0.000 title claims abstract description 7
- 230000002195 synergetic effect Effects 0.000 title claims abstract description 6
- 238000006555 catalytic reaction Methods 0.000 title claims description 5
- 239000007789 gas Substances 0.000 claims abstract description 15
- 238000000034 method Methods 0.000 claims abstract description 14
- 239000008188 pellet Substances 0.000 claims abstract description 11
- 239000002131 composite material Substances 0.000 claims abstract description 8
- 229910052802 copper Inorganic materials 0.000 claims abstract description 7
- 230000000593 degrading effect Effects 0.000 claims abstract description 7
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 6
- 230000003197 catalytic effect Effects 0.000 claims abstract description 3
- 238000005470 impregnation Methods 0.000 claims abstract description 3
- 229910052723 transition metal Inorganic materials 0.000 claims abstract description 3
- 239000000243 solution Substances 0.000 claims description 18
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 14
- 239000010453 quartz Substances 0.000 claims description 13
- 229910018072 Al 2 O 3 Inorganic materials 0.000 claims description 12
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 11
- 238000006243 chemical reaction Methods 0.000 claims description 11
- 238000005406 washing Methods 0.000 claims description 9
- 229910021642 ultra pure water Inorganic materials 0.000 claims description 8
- 239000012498 ultrapure water Substances 0.000 claims description 8
- 239000000463 material Substances 0.000 claims description 7
- 239000010949 copper Substances 0.000 claims description 6
- 238000001035 drying Methods 0.000 claims description 6
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 5
- 239000011889 copper foil Substances 0.000 claims description 5
- 229910001220 stainless steel Inorganic materials 0.000 claims description 5
- 239000010935 stainless steel Substances 0.000 claims description 5
- 230000004888 barrier function Effects 0.000 claims description 4
- 238000003756 stirring Methods 0.000 claims description 4
- 229920000742 Cotton Polymers 0.000 claims description 3
- 239000007864 aqueous solution Substances 0.000 claims description 3
- 238000001914 filtration Methods 0.000 claims description 3
- 238000011068 loading method Methods 0.000 claims description 3
- 238000010438 heat treatment Methods 0.000 claims description 2
- 238000012856 packing Methods 0.000 claims description 2
- 239000007787 solid Substances 0.000 claims description 2
- 238000004519 manufacturing process Methods 0.000 claims 3
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 abstract description 30
- 230000015556 catabolic process Effects 0.000 abstract description 12
- 238000006731 degradation reaction Methods 0.000 abstract description 12
- 230000008878 coupling Effects 0.000 abstract description 3
- 238000010168 coupling process Methods 0.000 abstract description 3
- 238000005859 coupling reaction Methods 0.000 abstract description 3
- 239000006227 byproduct Substances 0.000 abstract description 2
- 239000002440 industrial waste Substances 0.000 abstract description 2
- 230000015572 biosynthetic process Effects 0.000 abstract 1
- 238000005265 energy consumption Methods 0.000 abstract 1
- 229910002588 FeOOH Inorganic materials 0.000 description 10
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 6
- 230000000694 effects Effects 0.000 description 5
- 238000011049 filling Methods 0.000 description 5
- 238000010276 construction Methods 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- 238000002474 experimental method Methods 0.000 description 3
- 230000003647 oxidation Effects 0.000 description 3
- 238000007254 oxidation reaction Methods 0.000 description 3
- 238000007086 side reaction Methods 0.000 description 3
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 2
- AFCARXCZXQIEQB-UHFFFAOYSA-N N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CCNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 AFCARXCZXQIEQB-UHFFFAOYSA-N 0.000 description 2
- 239000013543 active substance Substances 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 230000005587 bubbling Effects 0.000 description 2
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 2
- 239000003446 ligand Substances 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
- 230000001105 regulatory effect Effects 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 239000012494 Quartz wool Substances 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 230000003213 activating effect Effects 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000007598 dipping method Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000012847 fine chemical Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000000543 intermediate Substances 0.000 description 1
- 239000013067 intermediate product Substances 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 229910000314 transition metal oxide Inorganic materials 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/88—Handling or mounting catalysts
- B01D53/885—Devices in general for catalytic purification of waste gases
-
- 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
- B01D53/32—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 by electrical effects other than those provided for in group B01D61/00
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/864—Removing carbon monoxide or hydrocarbons
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- 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
- B01J23/74—Iron group metals
- B01J23/745—Iron
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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
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- B01D2257/702—Hydrocarbons
- B01D2257/7027—Aromatic hydrocarbons
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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
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Abstract
The invention discloses a hydroxyl metal oxide catalyst, a preparation method and a method for degrading waste gas by coupling low-temperature plasma. The catalyst is characterized in that the catalyst is prepared by adopting an impregnation method, and the alumina pellets are used as a carrier to load the composite catalyst of nano hydroxyl metal oxide. Wherein, the transition metal element in the hydroxyl metal oxide is mainly Cu, fe, co, ni, zn, mn and other elements. The method realizes high-performance toluene degradation on the basis of low energy consumption and effectively inhibits the formation of byproducts. The plasma synergistic catalytic system based on the hydroxyl metal oxide constructed by the patent can realize high-performance waste gas treatment, is simple to operate and stable in system operation, and opens up a new idea for treating industrial waste gas.
Description
Technical Field
The invention relates to the field of discharge synergistic catalysts for waste gas treatment, in particular to a hydroxyl metal oxide catalyst for catalyzing and degrading industrial waste gas by synergistic discharge plasma, and a preparation method and application thereof.
Background
Volatile organic pollutants (VOCs) are a by-product of the rapid development of the industry in China, and have increasingly serious effects on the environment and human health. Currently, commonly used catalysts for degradation of VOCs are broadly classified into noble metal and transition metal oxides, with hydroxy metal oxides rarely being used for the treatment of VOCs. The hydroxyl metal oxide is a stable and effective degradation catalyst, and can be used for adsorbing pollutants and activating as an oxidant molecule due to the characteristics of large specific surface area, high hydroxyl density, multiple active sites and the like. In addition, the hydroxyl metal oxide does not contain an easily oxidized ligand, so that the possibility of side reaction is greatly reduced. The most main reason that the hydroxyl metal oxide is adopted as the catalyst for degrading waste gas in the patent is that compared with the traditional metal oxide, the hydroxyl metal oxide can remarkably improve the ozone oxidation capability. Ozone adsorbed on the surface of the hydroxyl metal oxide is decomposed into active oxygen with strong oxidizing property, and meanwhile, the conversion of hydrogen peroxide into OH is promoted, so that the conversion of target VOCs molecules and intermediate products is realized.
The plasma catalysis technology is formed by coupling non-thermal plasma and a catalyst, and has the advantages of mild reaction conditions, simple equipment, strong activation capability and the like. The packed bed reactor is a common DBD reactor, and partial discharge generated among medium particles in the packed bed improves average electron energy and further improves degradation rate. Common dielectric filling materials comprise glass, quartz, alumina, ceramic, ferroelectric materials and the like, the patent adopts alumina as a filling material of a filling bed, and hydroxyl metal oxide is attached to the surface of the alumina as a catalyst material.
Disclosure of Invention
The first object of the present invention is to provide a hydroxy metal oxide/gamma-Al for a packed bed DBD, which solves the problems of the prior art 2 O 3 A preparation method of a composite catalyst. The preparation method can obtain the composite catalyst which takes the alumina pellets as the carrier and uniformly adheres the hydroxyl metal oxide on the surface of the carrier. The hydroxyl metal oxide has a large specific surface area and hydroxyl groupsHigh density, multiple active reaction sites, no easily oxidized ligand, etc. The hydroxyl metal oxide can obviously improve the oxidation capability of ozone in the reaction, thereby improving the utilization rate of ozone in VOCs treatment.
The second object of the invention is to provide a construction method of the hydroxyl metal oxide catalyst cooperated with the packed bed plasma technology, which realizes the coupling of the packed medium in the packed bed and the hydroxyl metal oxide catalysis technology in the dielectric barrier discharge. The average electron energy is improved through partial discharge, more adsorption sites are provided for the reaction, more active substances are generated, and the probability of side reaction is reduced. The construction method has better activity and degradation effect under better discharge stability.
In order to achieve the first object, the present invention provides the following technical solutions: hydroxy metal oxide/gamma-Al for packed bed DBD 2 O 3 The preparation method of the composite catalyst is characterized in that the preparation process adopts an impregnation method, and specifically comprises the following steps:
s1, gamma-Al 2 O 3 Washing the carrier pellets with ultra-pure water, and washing the washed gamma-Al 2 O 3 The pellets are placed in a muffle furnace and dried and then baked.
S2, M (NO) 3 ) x (M is Cu, fe, co, ni, zn, mn) dissolved in ultra-pure water, and gamma-Al is added to the solution 2 O 3 And left to stand.
S3 adding H to the S2 solution 2 O 2 Stirring and heating the solution by adopting a magnetic stirrer; naOH is added to adjust the pH value.
And S4, filtering the solution in the step S3, washing and drying the filtered solid.
Is characterized in that the step 1 selects gamma-Al 2 O 3 The diameter of the pellets is 0.2-1 mm as a carrier; the temperature of the ultrapure water is 70-80 ℃, and the washing times are 8-10 times; the drying temperature of the muffle furnace is 100-120 ℃ and the drying time is 2-6 h; the roasting temperature of the muffle furnace is 425-500 ℃ and the roasting time is 2-10 h.
Its special feature isCharacterized in that M (NO) is added in step 2 3 ) x (M is Cu, fe, co, ni, zn, mn) with the concentration of 0.02-0.03 g/ml and the addition amount of 250-500 ml; the standing time is 12-24 h, and the standing temperature is 30-40 ℃.
Characterized in that H in step 3 2 O 2 The concentration of the solution is 25-35%, and the addition amount is 20-30 ml; the stirring time of the magnetic stirrer is 30-60 min, and the temperature is kept at 45-60 ℃; the concentration of NaOH is 0.4-0.5 mol/L, and the pH value of the aqueous solution is 9-10.
The method is characterized in that the muffle furnace temperature in the step 4 is 50-100 ℃ and the muffle furnace time is 2-6 h.
In order to achieve the second object, the present invention provides the following technical solutions: a construction method of a hydroxyl metal oxide catalyst cooperated packed bed plasma technology is characterized in that a cylindrical quartz tube is arranged on the shell of a cylinder, and a section of copper foil is wrapped on the outer side of the cylinder to serve as a grounding electrode; a high-voltage electrode made of stainless steel bars is placed on the axis of the quartz tube; quartz cotton is placed at two sides of the discharge area as a fixed material of a packed bed, and hydroxy metal oxide/gamma-Al is placed in the packed bed 2 O 3 And the transition metal element in the hydroxyl metal oxide is Cu, fe, co, ni, zn or Mn.
The method is characterized in that the length of the packing medium of the packed bed is 5-15 mm; the length of the copper foil (grounding electrode) is 5-15 mm; the inner diameter of the quartz tube is 2.5-4 mm, the outer diameter is 4-6 mm, and the thickness is 1.5-2 mm; the radius of the stainless steel rod high-voltage electrode is 1.5-2 mm.
In summary, the invention has the following beneficial effects:
the hydroxy metal oxide/gamma-Al prepared by the invention 2 O 3 The nanometer hydroxyl metal oxide in the composite catalyst is uniformly distributed in gamma-Al 2 O 3 A surface. gamma-Al 2 O 3 The pellets as packed bed material enhance the partial discharge effect created between the individual media particles, thereby increasing the average electron energy. While the active site on the surface of the hydroxy metal oxide promotes the reaction with O 3 Is a combination of (a) and (b). During the reaction, the surface of the packed bed is covered with hydroxy metalOxides, a large amount of O 3 The oxidation capability of ozone is obviously improved and the occurrence probability of side reactions is reduced by converting the ozone into active substances such as OH, O and the like.
The invention adopts a flexible method to couple the filling medium of the filling bed in the dielectric barrier discharge with the hydroxy metal oxide, has the advantages of low device cost, short degradation time, high degradation energy utilization rate and the like, and is suitable for small-scale fine chemical industry and large-scale application.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, a brief description of the drawings used in the examples or the description of the prior art will be given below.
FIG. 1 is FeOOH/gamma-Al prepared in example 1 2 O 3 XDR pattern of catalyst.
FIG. 2 is FeOOH/gamma-Al prepared in example 1 2 O 3 Catalyst pore size distribution map.
Fig. 3 is a DBD reactor apparatus diagram in example 2.
FIG. 4 is a graph of the effect of SEI on plasma-catalyzed degradation of toluene with or without FeOOH loading for (a) toluene degradation efficiency (b) energy yield for example 3.
Description of the preferred embodiments
Example 1: feOOH/gamma-Al 2 O 3 Preparation of the catalyst
The invention provides a FeOOH/gamma-Al 2 O 3 A method for preparing a catalyst comprising the steps of:
(1) Preparation of the solution: 6.0g of Fe (NO) 3 ) 3 ·9H 2 O was dissolved in 250ml of ultrapure water.
(2) Cleaning and roasting: taking gamma-Al with diameter of 0.5mm 2 O 3 The pellets were washed and dried at 80℃for 4 hours and then calcined at 425℃for 2 hours.
(3) Dipping: adding gamma-Al with proper weight to the solution obtained in the step (1) 2 O 3 The mixed solution was left at 40℃for 24 hours, and 30% strength H was added to the solution 2 O 2 20ml of solution and stirredFe(NO 3 ) 3 ·9H 2 O and H 2 O 2 The aqueous solution was mixed and heated to 55 ℃.
(4) Adjusting pH and filtering: the pH was adjusted to 9-10 with 0.5mol/L NaOH. Washing FeOOH/gamma-Al 2 O 3 And dried at 70 ℃.
The catalyst samples were subjected to x-ray diffraction (XRD) analysis by a Bruker D8 ADVANCE x-ray diffractometer, and the detection results are shown in FIG. 1. The FeOOH/gamma-Al is prepared 2 O 3 The pore size of the catalyst is shown in figure 2.
Example 2: experiment platform construction
The plasma reactor adopted by the invention is a laboratory self-made packed bed type coaxial cylinder DBD reactor. The reaction main body is made of a quartz glass tube with the length of 25cm, the outer diameter of 4mm and the inner diameter of 2.5mm, a stainless steel rod with the radius of 1.5mm is placed on the axis of the quartz tube and used as a high-voltage electrode of the reactor, and a copper foil with the width of 10mm is wrapped outside the quartz tube and used as a grounding electrode. In the example, ctp2000 low-temperature plasma experiment power supply provided by Nanjing Su Man electronic limited company is adopted as the power supply. The alternating current with the input of 220V and 50Hz is matched with a contact voltage regulator, the output voltage regulating range is 0-30 kV, and the output frequency regulating range is about 5-25 kHz. Placing 100mg of FeOOH/gamma-Al in the discharge region 2 O 3 And a catalyst, wherein quartz cotton fixed catalysts are arranged at two ends of the discharge area.
The toluene mixed gas in the invention is prepared as follows: the total gas flow rate was fixed at 600ml/min and all gas flows were controlled by mass flow controllers (MFC, D07, beijing seven star flow limited). The gas flow rate for bubbling the toluene solution was 30ml/min, and the background gas was N 2 The method comprises the steps of carrying out a first treatment on the surface of the Generating air by an air generator; the adjustment of the water vapor content was controlled by bubbling a certain amount of air into ultrapure water at room temperature, the sum of the flow rates of the standard air and the air containing a certain proportion of water vapor was 570ml/min, and all the gases were passed into a gas mixing bottle for gas mixing.
Referring to fig. 3, the dbd reactor device comprises a high-voltage electrode (1), a ground electrode (2), an air inlet (3), an air outlet (4), a quartz tube (5), quartz wool (6), feOOH/gamma-Al 2 O 3 A catalyst (7).
Example 3: feOOH/gamma-Al in different proportions 2 O 3 Catalyst degradation toluene comparison
Experiments were performed on the basis of example 2.
The experimental conditions are that the gas flow rate is 600ml/min, the toluene concentration is 2000ppm, no extra steam is generated, and the SEI variation range is 0.74-2.85. And comparing the influence of SEI on the catalytic degradation of toluene and the energy yield of the plasma under the condition of FeOOH load or not.
As shown in FIG. 4, the experimental results show that at SEI of 2.85kJ/L, the loading of FeOOH catalyst was increased from 0wt% to 8wt%, and toluene degradation efficiency was increased from 75.3% to 91.6%, so that FeOOH/gamma-Al was increased 2 O 3 The catalyst is beneficial for destroying toluene and organic intermediates.
Claims (8)
1. A dielectric barrier discharge synergistic hydroxy metal oxide catalysis method applied to waste gas treatment is characterized in that: the method employs a packed bed Dielectric Barrier Discharge (DBD) reaction apparatus; the catalyst is prepared by adopting an impregnation method, alumina pellets are used as a carrier to form a composite catalyst for loading nano hydroxyl metal oxide, and the composite catalyst is placed in a plasma discharge area to form a built-in plasma catalytic system.
2. The packed bed reaction device according to claim 1, adopting a coaxial cylindrical structure, characterized in that the shell of the cylinder is a cylindrical quartz tube, and a section of copper foil is wrapped on the outer side as a grounding electrode; a stainless steel rod is placed on the axis of the quartz tube to be used as a high-voltage electrode; quartz cotton is placed at two sides of the discharge area as a fixed material of a packed bed, and hydroxy metal oxide/gamma-Al is placed in the packed bed 2 O 3 And the transition metal element in the hydroxyl metal oxide is Cu, fe, co, ni, zn or Mn and the like.
3. A hydroxy metal oxide/gamma-Al according to claim 1 2 O 3 The preparation method of the composite catalyst is characterized in that the preparation process adopts dippingThe method specifically comprises the following steps:
s1, gamma-Al 2 O 3 Washing the carrier pellets with ultra-pure water, and washing the washed gamma-Al 2 O 3 The pellets are placed in a muffle furnace and dried and then baked.
S2, M (NO) 3 ) x (M is Cu, fe, co, ni, zn, mn) is dissolved in ultrapure water, and gamma-Al is added to the solution 2 O 3 And left to stand.
S3 adding H into the solution in S2 2 O 2 Stirring and heating the solution by adopting a magnetic stirrer; naOH is added to adjust the pH value.
And S4, filtering the solution in the step S3, washing and drying the filtered solid.
4. A process for preparing a catalyst for degrading exhaust gases according to claim 3, wherein step 1 is carried out by selecting γ -Al 2 O 3 The diameter of the pellets is 0.2-1 mm as a carrier; the temperature of the ultrapure water area is 70-80 ℃, and the washing times are 8-10 times; the drying temperature of the muffle furnace is 100-120 ℃ and the drying time is 2-6 h; the roasting temperature of the muffle furnace is 425-500 ℃ and the roasting time is 2-10 h.
5. A process for preparing a catalyst for degrading exhaust gases according to claim 3, wherein M (NO 3 ) x (M is Cu, fe, co, ni, zn, mn) with the concentration of 0.02-0.03 g/ml and the addition amount of 250-500 ml; the standing time is 12-24 h, and the standing temperature is 30-40 ℃.
6. A process for preparing a catalyst for degrading exhaust gas according to claim 3, wherein H in step 3 2 O 2 The concentration of the solution is 25-35%, and the addition amount is 20-30 ml; the stirring time of the magnetic stirrer is 30-60 min, and the temperature is kept at 45-60 ℃; the concentration of NaOH is 0.4-0.5 mol/L, and the pH value of the aqueous solution is 9-10.
7. The method for preparing a catalyst for degrading exhaust gas according to claim 3, wherein the muffle furnace temperature is 50-100 ℃ and the time is 2-6 h in the step 4.
8. The packed bed packing media of 5 to 15mm in length; the length of the copper foil (grounding electrode) is 5-15 mm; the inner diameter of the quartz tube is 2.5-4 mm, the outer diameter is 4-6 mm, and the thickness is 1.5-2 mm; the radius of the stainless steel rod high-voltage electrode is 1.5-2 mm.
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| CN202310546266.5A CN116371193A (en) | 2023-05-12 | 2023-05-12 | Hydroxyl metal oxide catalyst, preparation method and application thereof in plasma synergistic catalysis waste gas treatment |
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