CN112973351A - Ultralow emission device and method for dioxin in tail gas generated in thermal desorption process of organic contaminated soil - Google Patents
Ultralow emission device and method for dioxin in tail gas generated in thermal desorption process of organic contaminated soil Download PDFInfo
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- HGUFODBRKLSHSI-UHFFFAOYSA-N 2,3,7,8-tetrachloro-dibenzo-p-dioxin Chemical compound O1C2=CC(Cl)=C(Cl)C=C2OC2=C1C=C(Cl)C(Cl)=C2 HGUFODBRKLSHSI-UHFFFAOYSA-N 0.000 title claims abstract description 69
- 239000002689 soil Substances 0.000 title claims abstract description 54
- 238000000034 method Methods 0.000 title claims abstract description 53
- 238000003795 desorption Methods 0.000 title claims abstract description 47
- 230000008569 process Effects 0.000 title claims abstract description 23
- 239000007789 gas Substances 0.000 claims abstract description 91
- 230000003197 catalytic effect Effects 0.000 claims abstract description 66
- 238000001179 sorption measurement Methods 0.000 claims abstract description 54
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 51
- 230000003647 oxidation Effects 0.000 claims abstract description 50
- 239000000428 dust Substances 0.000 claims abstract description 44
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 43
- 239000012855 volatile organic compound Substances 0.000 claims abstract description 41
- LZKDJTLRGBUNTM-UHFFFAOYSA-N [O-2].[Ti+4].[Mo+4].[V+5] Chemical compound [O-2].[Ti+4].[Mo+4].[V+5] LZKDJTLRGBUNTM-UHFFFAOYSA-N 0.000 claims abstract description 30
- 238000002485 combustion reaction Methods 0.000 claims abstract description 21
- 238000010438 heat treatment Methods 0.000 claims abstract description 19
- 238000010791 quenching Methods 0.000 claims abstract description 16
- 238000002386 leaching Methods 0.000 claims abstract description 13
- 238000012544 monitoring process Methods 0.000 claims abstract description 10
- 239000007800 oxidant agent Substances 0.000 claims abstract description 10
- 230000001590 oxidative effect Effects 0.000 claims abstract description 10
- 238000012546 transfer Methods 0.000 claims abstract description 6
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims abstract description 4
- 239000003546 flue gas Substances 0.000 claims abstract description 4
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 3
- 239000003054 catalyst Substances 0.000 claims description 22
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 claims description 15
- 239000003463 adsorbent Substances 0.000 claims description 15
- 239000000460 chlorine Substances 0.000 claims description 15
- 229910052801 chlorine Inorganic materials 0.000 claims description 15
- 230000000694 effects Effects 0.000 claims description 15
- 229910000476 molybdenum oxide Inorganic materials 0.000 claims description 14
- 238000003860 storage Methods 0.000 claims description 13
- HSJPMRKMPBAUAU-UHFFFAOYSA-N cerium(3+);trinitrate Chemical compound [Ce+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O HSJPMRKMPBAUAU-UHFFFAOYSA-N 0.000 claims description 12
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 10
- PQQKPALAQIIWST-UHFFFAOYSA-N oxomolybdenum Chemical compound [Mo]=O PQQKPALAQIIWST-UHFFFAOYSA-N 0.000 claims description 10
- 229910052720 vanadium Inorganic materials 0.000 claims description 10
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims description 10
- 239000000243 solution Substances 0.000 claims description 9
- 238000006243 chemical reaction Methods 0.000 claims description 8
- 238000005470 impregnation Methods 0.000 claims description 8
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 7
- 239000004202 carbamide Substances 0.000 claims description 7
- 238000002360 preparation method Methods 0.000 claims description 7
- 230000000171 quenching effect Effects 0.000 claims description 7
- 239000003575 carbonaceous material Substances 0.000 claims description 6
- MIVBAHRSNUNMPP-UHFFFAOYSA-N manganese(2+);dinitrate Chemical compound [Mn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MIVBAHRSNUNMPP-UHFFFAOYSA-N 0.000 claims description 6
- 238000012986 modification Methods 0.000 claims description 6
- 230000004048 modification Effects 0.000 claims description 6
- 239000012047 saturated solution Substances 0.000 claims description 6
- 230000009123 feedback regulation Effects 0.000 claims description 5
- 206010022000 influenza Diseases 0.000 claims description 5
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- 239000011148 porous material Substances 0.000 claims description 4
- 238000000197 pyrolysis Methods 0.000 claims description 4
- 238000003756 stirring Methods 0.000 claims description 4
- 230000002195 synergetic effect Effects 0.000 claims description 4
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N titanium dioxide Inorganic materials O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 4
- 239000007864 aqueous solution Substances 0.000 claims description 3
- 238000001354 calcination Methods 0.000 claims description 3
- 238000000227 grinding Methods 0.000 claims description 3
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 3
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- 238000001816 cooling Methods 0.000 abstract description 4
- OKTJSMMVPCPJKN-BJUDXGSMSA-N carbon-11 Chemical compound [11C] OKTJSMMVPCPJKN-BJUDXGSMSA-N 0.000 description 5
- 238000005516 engineering process Methods 0.000 description 5
- 239000003344 environmental pollutant Substances 0.000 description 5
- 231100000719 pollutant Toxicity 0.000 description 5
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- 239000003795 chemical substances by application Substances 0.000 description 2
- 239000000356 contaminant Substances 0.000 description 2
- 238000007599 discharging Methods 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 238000005067 remediation Methods 0.000 description 2
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 2
- 229910000831 Steel Inorganic materials 0.000 description 1
- XHCLAFWTIXFWPH-UHFFFAOYSA-N [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] XHCLAFWTIXFWPH-UHFFFAOYSA-N 0.000 description 1
- 239000002156 adsorbate Substances 0.000 description 1
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- 230000000269 nucleophilic effect Effects 0.000 description 1
- 239000005416 organic matter Substances 0.000 description 1
- 235000011837 pasties Nutrition 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
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- 238000005406 washing Methods 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D50/00—Combinations of methods or devices for separating particles from gases or vapours
- B01D50/20—Combinations of devices covered by groups B01D45/00 and B01D46/00
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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
- B01D53/02—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 adsorption, e.g. preparative gas chromatography
- B01D53/04—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 adsorption, e.g. preparative gas chromatography with stationary adsorbents
-
- 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
- B01D53/8659—Removing halogens or halogen compounds
- B01D53/8662—Organic halogen compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C1/00—Reclamation of contaminated soil
- B09C1/06—Reclamation of contaminated soil thermally
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F27—FURNACES; KILNS; OVENS; RETORTS
- F27D—DETAILS OR ACCESSORIES OF FURNACES, KILNS, OVENS, OR RETORTS, IN SO FAR AS THEY ARE OF KINDS OCCURRING IN MORE THAN ONE KIND OF FURNACE
- F27D17/00—Arrangements for using waste heat; Arrangements for using, or disposing of, waste gases
- F27D17/008—Arrangements for using waste heat; Arrangements for using, or disposing of, waste gases cleaning gases
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2253/00—Adsorbents used in seperation treatment of gases and vapours
- B01D2253/10—Inorganic adsorbents
- B01D2253/102—Carbon
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- B01D2255/20707—Titanium
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- B01D2255/20723—Vanadium
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- B01D2255/20—Metals or compounds thereof
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- B01D2255/20769—Molybdenum
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Abstract
The invention discloses a device and a method for ultralow emission of dioxin in tail gas in the thermal desorption process of organic contaminated soil, which comprises a soil transfer unit for transporting the soil to be treated, a direct thermal desorption heating unit for heating the soil, a cyclone dust collector for primarily removing dust from the tail gas, a secondary combustion chamber for secondarily combusting the tail gas, a quench tower for cooling the secondarily combusted tail gas, a bag-type dust collector for further removing dust and an adsorption/catalytic oxidation tower, wherein the adsorption/catalytic oxidation tower adopts vanadium-molybdenum-titanium oxide as a catalytic oxidant for dioxin, converts the dioxin in the flue gas into VOCs, and adopts nitrogen-doped active carbon to adsorb the converted VOCs in the tail gas; the system also comprises a leaching tower for leaching and deacidifying, an exhaust chimney and a VOCs monitor for monitoring VOCs in the tail gas on line; the invention has better pertinence and flexibility, and can solve the problem of leaving polluted sites according to local conditions.
Description
Technical Field
The invention relates to the field of polluted soil remediation, is suitable for chlorine-containing organic polluted soil, and particularly relates to a device and a method capable of realizing ultralow emission of dioxin in tail gas in a direct thermal desorption process of the polluted soil.
Background
Aiming at a large amount of high-risk polluted soil generated by high-pollution enterprises such as steel, pesticides, chemical industry and the like, the thermal desorption technology is the most feasible treatment mode at present. The principle is that the polluted soil is heated in a direct or indirect heating mode, pollutants in the soil are decomposed and desorbed from the surface or pores of the soil to be converted into gas phase, and then the desorbed polluted tail gas is treated in modes of burning, adsorption or chemical reaction and the like. The thermal desorption technology has the advantages of wide pollutant treatment range, movable equipment, reusability of the repaired soil and the like, and is widely applied to ex-situ or in-situ remediation of organic polluted soil by developed countries such as Europe and America. The chlorine-containing organically-polluted soil inevitably causes tail gas dioxin emission in the thermal desorption process of the organically-polluted soil, so that secondary pollution is caused to the surrounding atmosphere. Meanwhile, the tail gas purification system of the existing polluted soil thermal desorption device has less attention to dioxin emission and cannot adapt to increasingly strict environmental protection standards. Therefore, attention should be paid to a device and a system for ultralow emission of dioxin in tail gas in the thermal desorption process of organic matter contaminated soil.
Disclosure of Invention
The invention aims to provide a device and a method for realizing ultralow emission of dioxin in tail gas in a direct thermal desorption process of polluted soil, aiming at the defects of the prior art. The device and the method provided by the invention are mainly used for directly carrying out thermal desorption on the chlorine-containing organic polluted soil, and ensuring ultralow emission of tail gas dioxin and volatile organic pollutants.
The purpose of the invention is realized by the following technical scheme: an ultralow emission device of dioxin in tail gas in a thermal desorption process of organic contaminated soil comprises a soil transfer unit, a direct thermal desorption heating unit, a cyclone dust collector, a secondary combustion chamber, a quench tower, a bag-type dust collector, an adsorption/catalytic oxidation tower, a leaching tower, a chimney and a VOCs monitor;
the soil transfer unit comprises a storage bin and a conveyor belt, the storage bin is filled with chlorine-containing organic polluted soil, and the storage bin is connected with the inlet end of the conveyor belt; the direct thermal desorption heating unit is a rotary kiln type heating structure and comprises a rotary kiln and a burner; the feeding end of the rotary kiln is connected with the output end of the conveyor belt and is communicated with the cyclone dust collector, and the thermal desorption tail gas is discharged from the feeding end of the rotary kiln and is introduced into the cyclone dust collector; the cyclone dust collector, the secondary combustion chamber, the quench tower, the bag-type dust collector and the adsorption/catalytic oxidation tower are sequentially connected, and tail gas generated after dust removal of the bag-type dust collector enters from the lower part of the adsorption/catalytic oxidation tower and is discharged from the upper part of the adsorption/catalytic oxidation tower.
The adsorption/catalytic oxidation tower is sequentially filled with vanadium-molybdenum-titanium oxide and nitrogen-doped activated carbon from bottom to top, the vanadium-molybdenum-titanium oxide is used as a catalytic oxidant of dioxin to convert the dioxin in the flue gas into VOCs, and the nitrogen-doped activated carbon is used as an adsorbent to adsorb the converted VOCs.
The VOCs monitor is used for monitoring the VOCs concentration of tail gas in front of and behind flues of the adsorption/catalytic oxidation tower and in front of the adsorbent behind the catalytic oxidant in the tower on line; and the tail gas discharged by the adsorption/catalytic oxidation tower is leached and deacidified by the leaching tower and then discharged by a chimney.
Further, the heating temperature of the rotary kiln is between 350 ℃ and 500 ℃.
Furthermore, the combustion temperature of the second combustion chamber is required to be above 850 ℃.
Further, the vanadium molybdenum titanium oxide is prepared by adding molybdenum oxide (MoO) in a moderate proportion in the vanadium-based catalystx) To thereby improve V2O5With the support TiO2The electronic effect between the two can enlarge the reaction temperature window and improve the catalytic oxidation of dioxinActivity and selectivity of the agent.
Furthermore, the preparation process of the vanadium molybdenum titanium oxide adopts an isometric impregnation method, and the method is characterized in that the pore volume of the catalyst carrier is equal to the volume of an impregnation solution, so that the effective components in the solution are uniformly dispersed on the surface of the carrier.
Further, the equal-volume impregnation method specifically comprises the following steps: dissolving manganese nitrate and cerium nitrate in water to prepare a saturated solution, weighing the same mass of vanadium-based catalyst and molybdenum oxide, adding the vanadium-based catalyst and molybdenum oxide into the saturated solution of manganese nitrate and cerium nitrate together, and fully stirring to obtain a paste. The paste was allowed to stand in air for 24 hours and then dried at 105 ℃ for 24 hours. And finally, grinding, sieving and calcining the sample to obtain the finished product of the vanadium-molybdenum-titanium oxide.
Furthermore, the nitrogen-doped activated carbon is prepared by using urea as a nitrogen source and carrying out doping modification through a mixed pyrolysis method, so that the surface polarity of the carbon material is improved, and the acting force between the carbon material and dioxin molecules is enhanced.
Further, the preparation method of the nitrogen-doped activated carbon takes columnar or powder activated carbon as a carrier, the columnar or powder activated carbon is immersed into urea saturated aqueous solution, stirred for 24 hours at the constant temperature of 80 ℃, filtered, washed and dried, and then N is added2And (5) heating and baking for 2 hours under the atmosphere protection, and storing for later use.
Furthermore, the VOCs monitor adopts a PID photo-ion sensor, and the tail gas data collected by the monitor is used for judging the operation effect of the adsorption/catalytic oxidation tower and carrying out feedback regulation.
The invention also provides an ultralow emission method of dioxin in tail gas in the thermal desorption process of the organic contaminated soil, which comprises the following specific steps:
(1) the chlorine-containing organic contaminated soil is transported to the rotary kiln through a bin and a conveyor belt, and is subjected to thermal desorption by a burner.
(2) And discharging thermal desorption tail gas from the feed end of the rotary kiln, introducing the thermal desorption tail gas into a cyclone dust collector, continuously introducing the thermal desorption tail gas into a secondary combustion chamber, and cooling the tail gas by a quench tower so as to inhibit the resynthesis of dioxin. And introducing the tail gas after the quenching tower into a bag-type dust remover for further tail gas dust removal.
(3) And introducing the tail gas subjected to dust removal into an adsorption/catalytic oxidation tower, introducing the tail gas from the lower part of the adsorption/catalytic oxidation tower, sequentially passing through vanadium-molybdenum-titanium oxide and nitrogen-doped activated carbon, and removing residual dioxin in the tail gas by adopting an adsorption method and a catalytic oxidation method in a synergistic manner, so that the deep removal of the dioxin in the tail gas is realized. And the VOCs concentration of tail gas in front of and behind flues of the adsorption/catalytic oxidation tower and in front of the adsorbent behind the catalytic oxidant in the tower is monitored on line by a VOCs monitor; used for judging the operation effect of the adsorption/catalytic oxidation tower and carrying out feedback regulation.
(4) And tail gas discharged from the upper end of the adsorption/catalytic oxidation tower is leached and deacidified by the leaching tower and then discharged from a chimney.
The invention has the beneficial effects that:
1) the invention designs a set of direct thermal desorption technical scheme aiming at chlorine-containing organic contaminated soil, and the technical scheme has better pertinence and flexibility and can solve the problem of leaving a contaminated site according to local conditions;
2) the adsorption/catalytic oxidation tower converts dioxin in tail gas into VOCs which are easier to treat through vanadium molybdenum titanium oxide, and then the VOCs are effectively removed through nitrogen-doped activated carbon, and the method is low in energy consumption, high in efficiency and high in feasibility;
3) for chlorine-containing organic contaminated soil, the invention adopts the scheme that the conventional tail gas dioxin emission reduction technology of a secondary combustion chamber and an emergency cooling tower is coupled with an adsorption/catalytic oxidation tower to realize the ultralow emission of tail gas dioxin. The effect of emission reduction of the tail gas pollutants is obviously superior to that of the prior art.
4) The invention carries out on-line monitoring on the device running condition through the VOCs monitor, can conveniently realize data acquisition, storage and real-time transmission, ensures the effectiveness and reliability of tail gas data, and effectively realizes the strict control of tail gas pollutant emission in the thermal desorption process.
Drawings
FIG. 1 is a schematic view of an ultralow emission system for directly thermally desorbing tail gas dioxin from chlorine-containing organic contaminated soil.
The reference numbers in the figures are: 1. a storage bin; 2. a conveyor belt; 3. a rotary kiln; 4. a burner; 5. a cyclone dust collector; 6. a second combustion chamber; 7. a quench tower; 8. a bag-type dust collector; 9. an adsorption/catalytic oxidation column; 10. vanadium molybdenum titanium oxide; 11. nitrogen-doped activated carbon; 12. leaching the tower; 13. a chimney; a VOCs monitor.
Detailed Description
The present invention will be described in further detail with reference to the accompanying drawings and specific embodiments.
As shown in fig. 1, the present invention provides an ultralow emission device of dioxin in tail gas generated in a thermal desorption process of chlorine-containing organic contaminated soil, which comprises a bin 1 and a conveyor belt 2 for receiving soil to be treated and transferring the soil to a rotary kiln, a rotary kiln 3 and a burner 4 for heating the soil, a cyclone 5 for primarily removing dust from the tail gas, a secondary combustion chamber 6 for secondarily combusting the tail gas, a quench tower 7 for cooling the tail gas after the secondary combustion, a bag-type dust remover 8 for further removing dust, an adsorption/catalytic oxidation tower 9 for purifying residual tail gas pollutants, a leaching tower 12 for leaching and deacidifying, and a chimney 13 for exhausting.
The soil transfer unit comprises a storage bin 1 and a conveyor belt 2, the storage bin 1 is filled with chlorine-containing organic polluted soil, and the storage bin 1 is connected with the inlet end of the conveyor belt 2; the direct thermal desorption heating unit is a rotary kiln type heating structure and comprises a rotary kiln 3 and a burner 4; the heating temperature of the rotary kiln is between 350 ℃ and 500 ℃. The feeding end of the rotary kiln 3 is connected with the output end of the conveyor belt 2 and is communicated with the cyclone dust collector 5, and thermal desorption tail gas is discharged from the feeding end of the rotary kiln 3 and is introduced into the cyclone dust collector 5 for primary dust removal; the cyclone dust collector 5, the secondary combustion chamber 6, the quench tower 7, the bag-type dust collector 8 and the adsorption/catalytic oxidation tower 9 are sequentially connected, the secondary combustion chamber 6 removes dioxin components in tail gas through secondary heating, and the combustion temperature is required to be above 850 ℃; the quenching tower 7 can rapidly cool the tail gas of the secondary combustion chamber 6, thereby inhibiting the resynthesis of dioxin. The tail gas after dust removal by the bag-type dust remover 8 enters from the lower part of the adsorption/catalytic oxidation tower 9 and is discharged from the upper part.
From the bottom to the bottom in the adsorption/catalytic oxidation tower 9Is sequentially filled with vanadium molybdenum titanium oxide 10 (V-Mo-TiO)2) And nitrogen-doped active carbon 11, and removing residual dioxin in the tail gas by adopting an adsorption method and a catalytic oxidation method in a synergistic manner. The vanadium molybdenum titanium oxide 10 is used as a catalytic oxidant of dioxin, the dioxin in the flue gas is converted into VOCs, and the nitrogen-doped activated carbon 11 is used as an adsorbent and used for adsorbing the converted VOCs. The vanadium molybdenum titanium oxide 10 is prepared by adding molybdenum oxide (MoO) in a medium proportion in a vanadium-based catalystx) To thereby improve V2O5With the support TiO2The reaction temperature window is enlarged by the electronic action between the two, and the activity and the selectivity of the dioxin catalyst are improved. The preparation process of the vanadium molybdenum titanium oxide 10 adopts an isometric impregnation method, and the method is characterized in that the pore volume of the catalyst carrier is basically equal to the volume of an impregnation solution, so that the effective components in the solution are uniformly dispersed on the surface of the carrier. The preparation process specifically comprises the steps of dissolving manganese nitrate and cerium nitrate in water to prepare a saturated solution, weighing the same mass of the vanadium-based catalyst and molybdenum oxide, adding the vanadium-based catalyst and the molybdenum oxide into the saturated solution of the manganese nitrate and the cerium nitrate together, and fully stirring the mixture to obtain a pasty paste. The paste was allowed to stand in air for 24 hours and then dried at 105 ℃ for 24 hours. And finally, grinding, sieving and calcining the sample to obtain the finished product of the vanadium-molybdenum-titanium oxide. The nitrogen-doped activated carbon 11 is prepared by using urea as a nitrogen source and performing doping modification through a mixed pyrolysis method, so that the surface polarity of the carbon material is improved, and the acting force between the carbon material and dioxin molecules is enhanced. The preparation method of the nitrogen-doped activated carbon 11 takes columnar or powdery activated carbon as a carrier, and the columnar or powdery activated carbon is immersed in urea saturated aqueous solution and stirred for 24 hours at the constant temperature of 80 ℃. Filtering, washing, drying, and adding N2And (5) heating and baking for 2 hours under the atmosphere protection, and storing for later use.
The VOCs monitor 14 adopts a PID photo-ion sensor, can carry out on-line monitoring on the concentration of VOCs in tail gas at the front and rear flues of the adsorption/catalytic oxidation tower 9 and the front position of the adsorbent behind the catalytic oxidation agent in the tower, and has the characteristics of convenience in installation, high measurement precision, good reliability, high response speed and the like. Meanwhile, the tail gas data collected by the VOCs monitor 14 can be used for judging the operation effect of the adsorption/catalytic oxidation tower and performing feedback regulation.
The tail gas discharged from the adsorption/catalytic oxidation tower 9 is leached and deacidified by a leaching tower 12 and then discharged from a chimney 13.
Chlorine-containing organically-polluted soil inevitably causes tail gas dioxin emission in the thermal desorption process of the organically-polluted soil. The conventional tail gas dioxin emission reduction technology adopts the reburning of a secondary combustion chamber to remove tail gas dioxin components, and the quenching tower quenches to inhibit the resynthesis of the dioxin. On the basis, the residual dioxin in the tail gas is removed by adopting a catalytic oxidation method and an adsorption method in a synergistic manner, so that the ultralow emission of the dioxin in the tail gas is realized.
The loading of transition metal oxides onto catalyst supports is a common way of catalyst preparation. Related studies show that V2O5Has better activity on the degradation of dioxin. Wherein, the V ═ O group in the vanadium oxide can realize nucleophilic adsorption on dioxin molecules, and then a series of oxidation reactions are carried out to convert the dioxin molecules into VOCs with smaller molecular sizes. Therefore, the invention adopts vanadium molybdenum titanium oxide (V-Mo-TiO)2) As a catalytic oxidant for dioxin, molybdenum oxide (MoO) is added in a proper amount to a vanadium-based catalystx) Thereby improving V2O5With the support TiO2The reaction temperature window is enlarged by the electronic action between the two, and the activity and the selectivity of the dioxin catalyst are improved. The catalytic test shows that the catalytic removal efficiency of the vanadium molybdenum titanium oxide is increased along with the increase of the reaction temperature, when the reaction temperature is 150 ℃, the catalytic removal efficiency can reach 88 percent, and when the reaction temperature is 170 ℃, the catalytic removal efficiency is 91 percent.
In the invention, after dioxin in the tail gas is converted into VOCs, the VOCs in the tail gas are adsorbed by a proper adsorbent, and the quality of the adsorbent is not only related to the adsorption quantity, but also related to the acting force of the adsorbent and dioxin molecules. Researches show that the surface polarity of the activated carbon material can be improved by a nitrogen doping modification technology, so that the molecular acting force between the adsorbent and the adsorbate is enhanced, and the adsorption effect is improved. Therefore, the nitrogen-doped activated carbon is used as an adsorbent, urea is used as a nitrogen source, and the nitrogen-doped activated carbon is prepared by carrying out doping modification through a mixed pyrolysis method.
In addition, online monitoring of contaminants is an important ring to achieve effective control of contaminants. After tail gas dioxin is catalyzed into VOCs, the method can indirectly realize real-time monitoring on dioxin emission through monitoring of catalytic products. The VOCs monitor is based on a PID photo-ion sensor, and ionizes VOCs in the air by using an ultraviolet lamp as a light source, but the basic component N in the air2、O2、CO2Etc. are not ionized. And the electrons generated by ionization and positively charged ions can form weak current under the action of an electric field, and the content of VOCs can be reflected by detecting the current intensity.
Based on the principle and the device provided by the invention, the invention also provides a method for ultralow emission of dioxin in tail gas in the thermal desorption process of chlorine-containing organically-polluted soil, as shown in figure 1, the chlorine-containing organically-polluted soil is moved into a rotary kiln 3 through a storage bin 1 and a conveyor belt 2, and is thermally desorbed by a burner 4. And discharging the thermal desorption tail gas from the feed end, introducing the thermal desorption tail gas into a cyclone dust collector 5, then continuously introducing the thermal desorption tail gas into a secondary combustion chamber 6, and removing most dioxin components in the tail gas through high-temperature incineration. And then the tail gas is rapidly cooled by a quenching tower 7, so that the resynthesis of the dioxin is inhibited. And introducing the tail gas after the quenching tower 7 into a bag-type dust remover 8 for further tail gas dust removal. And introducing the tail gas subjected to dust removal into an adsorption/catalytic oxidation tower 9, wherein the tail gas enters from the lower part of the device and sequentially passes through nitrogen-doped activated carbon 11 and vanadium-molybdenum-titanium oxide 10, so that the deep removal of dioxin in the tail gas is realized. Finally, the tail gas is discharged from a chimney 13 after being leached and deacidified by the leaching tower 12. The VOCs monitor 14 detects the concentration of VOCs in the exhaust gas in front of and behind the flue of the adsorption/catalytic oxidation tower 9 and in front of the adsorbent behind the catalyst in the tower by using a PID photo-ion sensor. The monitoring data of the front flue of the adsorption/catalytic oxidation tower 9 and the rear position of the catalyst in the tower can reflect the catalytic oxidation effect of vanadium molybdenum titanium oxide on dioxin, and the monitoring data of the rear flue of the adsorption/catalytic oxidation tower 9 and the rear position of the catalyst in the tower can reflect the adsorption effect of nitrogen-doped activated carbon on VOCs. The catalyst and the adsorption in the adsorption/catalytic oxidation tower 9 have certain service time limit, and when the catalytic effect of the vanadium-molybdenum-titanium oxide or the adsorption effect of the nitrogen-doped active carbon is reduced to a certain value, a worker can find and replace the catalyst or the adsorbent in time through the VOCs online monitor, so that the ultralow emission of dioxin in the tail gas of the thermal desorption device is ensured.
It should be noted that the above-mentioned list is only the specific embodiment of the present invention. It is obvious that the present invention is not limited to the above embodiments, but many variations are possible. All modifications which can be derived or suggested by a person skilled in the art from the disclosure of the present invention are to be considered within the scope of the invention.
Claims (10)
1. The ultralow emission device of dioxin in tail gas of the thermal desorption process of organic contaminated soil is characterized by comprising a soil transfer unit, a direct thermal desorption heating unit, a cyclone dust collector (5), a secondary combustion chamber (6), a quench tower (7), a bag-type dust collector (8), an adsorption/catalytic oxidation tower (9), a leaching tower (12), a chimney (13) and a VOCs monitor (14);
the soil transfer unit comprises a storage bin (1) and a conveyor belt (2), chlorine-containing organic polluted soil is filled in the storage bin (1), and the storage bin (1) is connected with the inlet end of the conveyor belt (2); the direct thermal desorption heating unit is a rotary kiln type heating structure and comprises a rotary kiln (3) and a burner (4); the feeding end of the rotary kiln (3) is connected with the output end of the conveyor belt (2) and is communicated with the cyclone dust collector (5), and thermal desorption tail gas is discharged from the feeding end of the rotary kiln (3) and is introduced into the cyclone dust collector (5); the cyclone dust collector (5), the secondary combustion chamber (6), the quench tower (7), the bag-type dust collector (8) and the adsorption/catalytic oxidation tower (9) are sequentially connected, tail gas generated after dust removal of the bag-type dust collector (8) enters from the lower part of the adsorption/catalytic oxidation tower (9), and is discharged from the upper part of the adsorption/catalytic oxidation tower.
The adsorption/catalytic oxidation tower (9) is sequentially filled with vanadium molybdenum titanium oxide (10) and nitrogen-doped activated carbon (11) from bottom to top, the vanadium molybdenum titanium oxide (10) is used as a catalytic oxidant of dioxin to convert the dioxin in flue gas into VOCs, and the nitrogen-doped activated carbon (11) is used as an adsorbent to adsorb the converted VOCs.
The VOCs monitor (14) is used for carrying out on-line monitoring on the VOCs concentration of tail gas in front and rear flues of the adsorption/catalytic oxidation tower (9) and in front of a catalytic oxidant rear adsorbent in the tower; and tail gas discharged by the adsorption/catalytic oxidation tower (9) is leached and deacidified by a leaching tower (12) and then discharged by a chimney (13).
2. The ultra-low dioxin discharge device used in the thermal desorption process of organically-polluted soil according to claim 1, wherein the heating temperature of the rotary kiln (3) is between 350 ℃ and 500 ℃.
3. The ultralow emission device of dioxin during the thermal desorption process of organically-polluted soil according to claim 1, characterized in that the combustion temperature of the second combustion chamber (6) is required to be above 850 ℃.
4. The ultra-low dioxin emission device in thermal desorption process of organically-polluted soil as claimed in claim 1, wherein the vanadium-molybdenum-titanium oxide (10) is prepared by adding molybdenum oxide (MoO) in a medium proportion in a vanadium-based catalystx) To thereby improve V2O5With the support TiO2The reaction temperature window is enlarged, and the activity and the selectivity of the dioxin catalytic oxidant are improved.
5. The ultra-low dioxin emission device from thermal desorption process of organically-polluted soil according to claim 1, characterized in that the vanadium molybdenum titanium oxide (10) is prepared by an equal volume impregnation method, which is characterized in that the pore volume of the catalyst carrier is equal to the volume of the impregnation solution, so as to ensure that the effective components in the solution are uniformly dispersed on the surface of the carrier.
6. The ultralow emission device of dioxin in the thermal desorption process of organic contaminated soil according to claim 5, wherein the equivalent-volume impregnation method is specifically as follows: dissolving manganese nitrate and cerium nitrate in water to prepare a saturated solution, weighing the same mass of vanadium-based catalyst and molybdenum oxide, adding the vanadium-based catalyst and molybdenum oxide into the saturated solution of manganese nitrate and cerium nitrate together, and fully stirring to obtain a paste. The paste was allowed to stand in air for 24 hours and then dried at 105 ℃ for 24 hours. And finally, grinding, sieving and calcining the sample to obtain the finished product of the vanadium-molybdenum-titanium oxide.
7. The ultralow emission device of dioxin during the thermal desorption process of organic contaminated soil according to claim 1, characterized in that the nitrogen-doped activated carbon (11) is prepared by doping modification through a mixed pyrolysis method by using urea as a nitrogen source, so as to improve the surface polarity of the carbon material and enhance the acting force between the carbon material and dioxin molecules.
8. The ultralow emission device of dioxin during the thermal desorption process of organically-polluted soil according to claim 7, characterized in that the preparation method of the nitrogen-doped activated carbon (11) is to immerse columnar or powdered activated carbon as a carrier in a urea saturated aqueous solution, stir the solution at a constant temperature of 80 ℃ for 24 hours, filter, wash and dry the solution, and then add N to the solution2And (5) heating and baking for 2 hours under the atmosphere protection, and storing for later use.
9. The ultralow emission device of dioxin in the thermal desorption process of organically-polluted soil according to claim 1, characterized in that the VOCs monitor (14) employs a PID photo-ion sensor, and the tail gas data collected by the VOCs monitor (14) is used for judging the operation effect of the adsorption/catalytic oxidation tower (9) and performing feedback regulation.
10. The emission method of the ultralow emission device of dioxin in the thermal desorption process of the organically-polluted soil according to any one of claims 1 to 9, characterized by comprising the following specific steps:
(1) the chlorine-containing organic contaminated soil is transferred into a rotary kiln (3) through a storage bin (1) and a conveyor belt (2), and is subjected to thermal desorption by a burner (4).
(2) And thermal desorption tail gas is discharged from the feed end of the rotary kiln (3), is introduced into the cyclone dust collector (5), is continuously introduced into the secondary combustion chamber (6), and is cooled by the quenching tower (7), so that the resynthesis of dioxin is inhibited. And introducing the tail gas after the quenching tower (7) into a bag-type dust remover (8) for further tail gas dust removal.
(3) And introducing the tail gas subjected to dust removal into an adsorption/catalytic oxidation tower (9), introducing the tail gas from the lower part of the adsorption/catalytic oxidation tower (9), sequentially passing through a vanadium-molybdenum-titanium oxide (10) and nitrogen-doped active carbon (11), and removing residual dioxin in the tail gas by adopting an adsorption method and a catalytic oxidation method in a synergistic manner, thereby realizing deep removal of the dioxin in the tail gas. And the VOCs concentration of tail gas in front of and behind flues of the adsorption/catalytic oxidation tower (9) and in front of the adsorbent behind the catalytic oxidant in the tower is monitored on line by a VOCs monitor (14); used for judging the operation effect of the adsorption/catalytic oxidation tower and carrying out feedback regulation.
(4) The tail gas discharged from the upper end of the adsorption/catalytic oxidation tower (9) is leached and deacidified by the leaching tower (12) and then discharged from a chimney (13).
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