CN103272839A - Low-temperature plasma processing device and method for persistent organic pollutants in soil - Google Patents
Low-temperature plasma processing device and method for persistent organic pollutants in soil Download PDFInfo
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- CN103272839A CN103272839A CN2013101576165A CN201310157616A CN103272839A CN 103272839 A CN103272839 A CN 103272839A CN 2013101576165 A CN2013101576165 A CN 2013101576165A CN 201310157616 A CN201310157616 A CN 201310157616A CN 103272839 A CN103272839 A CN 103272839A
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- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
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Abstract
A low-temperature plasma processing device and a method for persistent organic pollutants in soil are disclosed. The device comprises a reaction kettle and a reaction stage. The reaction kettle consists of a reaction kettle container provided with a gas inlet and a gas outlet, and a reaction kettle cover plate arranged on the reaction kettle container. The reaction stage comprises an insulation plate, a conductive base, a low-temperature plasma power supply and a fan; the conductive base is provided with a strut, a ground electrode and a lower binding post, the insulation plate is arranged on the strut and provided with a high voltage electrode and an upper binding post, the high voltage electrode and the ground electrode are arranged oppositely, the fan is arranged toward the electrodes, the upper binding post is connected with the low-temperature plasma power supply, the lower binding post is connected with a ground wire, and the reaction kettle is arranged between the high voltage electrode and the ground electrode. The processing device is simple in operation, high in pollutant removal efficiency, small in device investment and low in processing cost, and is suitable for a small-scale test on the recovery of persistent organic pollution soil.
Description
Technical field
The invention belongs to organic polluted soil recovery technique field, be specifically related to a kind of apparatus for low-temperature plasma treatment and method of soil persistent organic pollutant using.
Background technology
Persistence organic pollutant (Persistent Organic Pollutants is called for short POPs) mainly is divided into three major types: the byproduct (dioxin and furans) in pesticide (drinox, Niran, DDT etc.), industrial chemical (Polychlorinated biphenyls and hexachloro-benzene) and the production.In recent years, pesticide and industrial chemical are widely used in China's industrial and agricultural production.Because these materials have strong toxicity, difficult, the easily enrichment of degraded, the most of agricultural land soil of China and industrial land can detect all that it is residual, and human security is brought potential hazard.Therefore, cause that people pay close attention to widely.
POPs refer to by various surrounding mediums (atmosphere, water, organism etc.) can long-distance migration and long-term existence in environment, have extended residual, biological accumulation, half volatile and high toxicity, human health and environment are had the natural of serious harm or artificial synthetic organic pollution materials.After POP enters environment by all means, can cause the ecosystem to seriously influence and destroy, correlative study shows that organism is exposed to POPs can cause that also dysgenesia, deformity, organ increase phenomenons such as body death.Harm mainly contains to human body: a class is the influence to children's birth weight, the obstacle of skeleton development and the disorder of metabolism; Second class is to nervous system, the disorder of notice, immune inhibition; The 3rd class is the harm to reproductive system.The 4th class is carcinogenic.Therefore, must carry out properly and the science disposal the soil after the persistence organic pollutant pollution, to guarantee its safety.
At present, the recovery technique of persistence organic pollutant commonly used mainly contains: high temperature incineration, cement kiln disposal, thermal desorption, mechanochemistry dehalogenation, vitrifying technology etc., yet high temperature incineration and cement kiln disposal technology require high, and have the potential danger that forms secondary pollution, thermal desorption, mechanochemistry dehalogenation and vitrifying technical finesse cost are higher.
In the atmos low-temperature plasma technical gas discharge plasma, high vibration excited state or electron excitation metastable state N that electronics and airborne nitrogen, oxygen, hydrone collision generate
2Material, strong oxidizing property material, these species act on pollutant, finally generate carbon dioxide and water, have opened up new approach for removing noxious pollutant at low temperatures.Dielectric barrier discharge is a kind of mode that produces low temperature plasma, it refers to dielectric is inserted a kind of nonequilibrium state gas discharge of discharge space, when applying sufficiently high alternating voltage between two electrodes, interelectrode gas is understood breakdown and is produced discharge, has namely produced dielectric barrier discharge.
What patent JP2002153834 adopted is after pending soil is heated to uniform temperature, carry out the method for Low Temperature Plasma Treating after forcing pollutant in the pending soil to be overflowed in the gas mode, this method is obviously destroyed the original physicochemical property of soil because of heat treated.What patent JP2004283684 adopted is after the volatile organic contaminant extracting in the soil dusty gas to be carried out the method for Low Temperature Plasma Treating.Yet these two kinds of methods relatively are applicable to volatile organic contaminant contaminated soil and organic pollution and pollute short soil of time, for handling persistence organic pollutant certain limitation arranged.And these two kinds for the treatment of system equipment investments are bigger, and processing cost is higher.
Summary of the invention
The technical problem that solves: the application provides a kind of apparatus for low-temperature plasma treatment and method with good repairing effect at severe persistent organism contaminated soil (especially place contaminated soil).
Technical scheme: a kind of apparatus for low-temperature plasma treatment of soil persistent organic pollutant using, comprise reactor and reaction bench, described reactor is made up of reactor container and reactor cover plate, described reactor container is provided with air inlet and gas outlet, and the reactor cover plate is located on the reactor container; Reaction bench comprises insulation board, conductive seat, low-temperature plasma electrical source and fan, conductive seat is provided with support bar, insulation board is located on the support bar, insulation board is provided with high-field electrode and last binding post, and conductive seat is provided with earth electrode and following binding post, and high-field electrode and earth electrode are oppositely arranged, fan is towards the electrode setting, last binding post is connected with low-temperature plasma electrical source, and following binding post is connected with ground wire, and reactor is located between high-field electrode and the earth electrode.
Described support bar is provided with the insulation board arrangement for adjusting height, and described arrangement for adjusting height is nut.
Two opposite flanks of described insulation board are provided with adjusting nut, in order to the fixation reaction still.
Described high-field electrode and earth electrode are cylinder, and the cylinder side is provided with one group of groove.
Described reactor is made up of quartz reaction kettle cover plate and reactor container, and described reactor container is made of quartzy annulus and stainless steel base plate, offers two holes on the quartzy annulus, is connected with quartz ampoule on the hole.
Described low-temperature plasma electrical source power output is 0～2kW, frequency-tuning range 5～30kHz, and the output voltage adjustable range is 0～30kV.
Described device is handled the method for soil persistent organic pollutant using, and step is: the first step, and the natural air drying contaminated soil after the screening is put into reactor, and make it evenly to cover the reactor bottom; Second step placed reactor between the electrode, and behind the connection power supply, dielectric barrier discharge produces low temperature plasma and the persistence organic pollutant reaction also makes it to remove.
When handling gesarex polluted soil, low-temperature plasma electrical source power output 1kW, processing time 20min, atmospherical discharges atmosphere, soil particle diameter＜1mm.
When handling polycyclic aromatic hydrocarbon pollution, low-temperature plasma electrical source power output 1kW, processing time 15min, atmospherical discharges atmosphere, soil particle diameter＜1mm.
Beneficial effect: the apparatus for low-temperature plasma treatment of soil persistent organic pollutant using of the present invention and method, utilize existing O in the reactor
2, N
2High energy electron in the low temperature plasma that produces with low amounts of water equimolecular and dielectric barrier discharge bumps, and generates OH, H, O, O
3, HO
2Etc. active free radical, these free radicals and contaminant molecule produce a series of reaction and produce free of contamination CO
2And H
2O.This treating apparatus is simple to operate, removes pollutant efficient height, and equipment investment is little, and processing cost is low, is applicable to the small-scale test of persistency organic contaminant soil remediation.
Description of drawings
Fig. 1 is the apparatus for low-temperature plasma treatment structural representation of soil persistent organic pollutant using of the present invention;
Fig. 2 is reaction of low temperature plasma still structural representation among Fig. 1;
Fig. 3 is that the processing time is to the influence of total DDT concentration;
Fig. 4 be the processing time to o, p'-DDE, p, p'-DDE, o, p'-DDT and p, the influence of p'-DDT concentration;
Fig. 5 is that the processing time is to the influence of total polycyclic aromatic hydrocarbon and benzo [a] pyrene concentration.
Reactor container 1 among the figure, reactor cover plate 2, earth electrode 3, support bar 4, nut 5, high-field electrode 6, insulation board 7, nut 8, air inlet 9, gas outlet 10, last binding post 11, low-temperature plasma electrical source 12, conductive seat 13, following binding post 14, fan 15.
The specific embodiment
Following examples further specify content of the present invention, but should not be construed as limitation of the present invention.Without departing from the spirit and substance of the case in the present invention, modification and replacement to the inventive method, step or condition are done all belong to scope of the present invention.
If do not specialize the conventional means that used technological means is well known to those skilled in the art among the embodiment.
Embodiment 1:
The Low Temperature Plasma Treating method of soil persistent organic pollutant using of the present invention mainly is: the first step, natural air drying contaminated soil after the screening is put into reactor, and make it evenly to cover reactor container 1 bottom, again reactor cover plate 2 is covered on reactor container 1; Second step placed reactor on the earth electrode 3, and the height of regulating high-field electrode 6 by the nut 5 of rotation stainless steel support bar 4 makes it to fit tightly with reactor, and it is fixing that the nut 8 of tightening insulation board 7 both sides again makes it to keep; The 3rd step, build deacration other discharge atmosphere in addition if desired, required atmosphere can be entered reaction system by reactor air inlet 9,10 discharges through the gas outlet again; The 4th step, last binding post 11 on the insulation board 7 of polytetrafluoroethylene (PTFE) material is joined with low-temperature plasma electrical source 12, following binding post 14 on the stainless steel conductive seat 13 is joined with ground wire, open low-temperature plasma electrical source 12 and power output and be set to 1kW, open cooling fan 15; The 5th step kept good discharge condition, made dielectric barrier discharge produce existing O in low temperature plasma and the reaction system
2, N
2Generate OH, H, O, O with the low amounts of water equimolecular
3, HO
2Etc. active free radical, until these free radicals and contaminant molecule complete reaction, regulate again and close low-temperature plasma electrical source 12 after power is lower than 200W.
Embodiment 2:
A kind of apparatus for low-temperature plasma treatment of soil persistent organic pollutant using, comprise reactor and reaction bench, described reactor is made up of reactor container 1 and reactor cover plate 2, and described reactor container is provided with air inlet 9 and gas outlet 10, and reactor cover plate 2 is located on the reactor container 1; Reaction bench comprises insulation board 7, conductive seat 13, low-temperature plasma electrical source 12 and fan 15, conductive seat 13 is provided with support bar 4, insulation board 7 is located on the support bar 4, insulation board 7 is provided with high-field electrode 6 and last binding post 11, conductive seat 13 is provided with earth electrode 3 and following binding post 14, high-field electrode 6 and earth electrode 3 are oppositely arranged, fan 15 is towards the electrode setting, last binding post 11 is connected with low-temperature plasma electrical source 12, following binding post 14 is connected with ground wire, and reactor is located between high-field electrode 6 and the earth electrode 3.Described support bar 4 is provided with the insulation board arrangement for adjusting height, and described arrangement for adjusting height is nut 5.Two opposite flanks of described insulation board 7 are provided with adjusting nut 8, in order to the fixation reaction still.Described high-field electrode 6 and earth electrode 3 are cylinder, and the cylinder side is provided with one group of groove.Described reactor is made up of quartz reaction kettle cover plate and reactor container, and described reactor container is made of quartzy annulus and stainless steel base plate, offers two holes on the quartzy annulus, is connected with quartz ampoule on the hole.Low-temperature plasma electrical source (CTP-2000K, Nanjing Rong Man Electronics Co., Ltd.) power output is 0～2kW, frequency-tuning range 5～30kHz, and the output voltage adjustable range is 0～30kV.
Embodiment 3:
With embodiment 2, a kind of apparatus for low-temperature plasma treatment of soil persistent organic pollutant using comprises low-temperature plasma electrical source, two stainless steel discharge electrodes, reactor and external cooling fans.Described reactor places between two stainless steel electrodes, and the three fits tightly.Described low-temperature plasma electrical source power output is 0～2kW, frequency-tuning range 5～30kHz, and the output voltage adjustable range is 0～30kV.Described sparking electrode is the stainless steel cylinder of diameter 150mm, thickness 26mm, the electrode sidewall periphery design 5 road grooves, the surface area that this design has increased electrode is beneficial to electrode heat radiation in the discharge process.Described sparking electrode is made of high-field electrode and earth electrode, wherein be fixed on the high-field electrode of polytetrafluoroethylene (PTFE) material insulation board by the anodal low-temperature plasma electrical source that connects, the earth electrode that is fixed on the stainless steel base links to each other with ground wire by negative terminal.The teflon insulation plate by two threaded stainless steel columns be supported on the stainless steel base directly over.Reactor comprises that a container and a diameter are that 214mm, thickness are the quartzy cover plate of 3mm, and this container is that 214mm, internal diameter are that 150mm, thickness are that the quartzy annulus of sheet of 8mm and diameter are that 168mm, thickness are that the stainless-steel sheet of 3mm is bonded up and down by a slice external diameter.In the quartzy annulus both sides of container, the aperture that to have a diameter separately be 6mm, this aperture is apart from quartzy upper surface 1mm, and the quartz round tube of an external bending.This design can be used for feeding the required all gases of experimental design in reactor, thereby builds different discharge of plasma in low temperature atmosphere.Described external cooling fan is NMB2110KL-03B-B65, power 3.6W, is used for the stainless steel electrode cooling.
Embodiment 4: adopt embodiment 3 equipment to investigate the processing time to the influence of DDT (DDTs) clearance
For trying soil: pick up from the discarded production site of Zhangjiakou DDT, its basic physical and chemical is as shown in table 1.Pollutant in soil mainly comprises 6 kinds of DDT and derivative thereof etc., and soil is crossed 20 orders (1mm) sieve behind natural air drying, standby.
Table 1 is for the basic physical and chemical of examination soil
Basic parameter arranges: discharge power 1kW, soil particle diameter＜1mm, atmospherical discharges atmosphere, frequency 50Hz and voltage 220V(standard line voltage); Processing time: establish 0,1,5,10,15,20,25,30,40min totally 9 levels, each level is done 4 repetitions.Soil is crossed 60 mesh sieves after the low temperature plasma post processing, uses for analyzing DDTs content.
Interpretation of result:
As shown in Figure 3, along with the increase in processing time, ∑ DDT concentration is remarkable downward trend.In 0～15min time period, ∑ DDT descends comparatively slow; Between 15～20min, ∑ DDT is from 207.6mgkg
-1Drop to 9.23mgkg
-1Behind the 20min, downward trend is mild.When the processing time was 20min, the clearance of ∑ DDT can reach 98.1%.
For different component pollutant levels variation tendency as shown in Figure 4.Wherein, p, p'-DDE, o, p'-DDT and p, p'-DDT concentration all significantly descends along with the increase in processing time, and o, p'-DDE concentration then is to rise to some extent in the incipient stage, descends gradually behind the 5min.Each component downward trend all tends towards stability behind the 20min, and its concentration almost no longer changes.As seen from Figure 4, the processing time, DDTs concentration sharply descended when being 20min, slightly descended afterwards, and clearance is 95.3%～99.9%.
As shown in Table 2, when the processing time is 20min, o, p'-DDD and p, the clearance of p'-DDD are 99.3% and 98.1%.
Table 2 processing time is to the influence of o p'-DDD and p p'-DDD removal effect
The result shows, when processing time 5min, and o, p'-DDE concentration reaches maximum, is remarkable decline subsequently, and this may be because the free radical, excited atom, excited state molecule isoreactivity material and the finite energy that produce in 0～5min, can not make o, the p'-DDT complete oxidation generates CO
2, HO
2Deng, generate o, p'-DDE thereby only have portion C-H key and C-Cl key that fracture takes place.And p, p'-DDE concentration does not obviously earlier increase the back downward trend, may be because the p in the soil yet, and the p'-DDT relative concentration is lower, and the p of generation, p'-DDE are also lower thereby variation tendency is not obvious.Be 20min when the processing time, DDTs clearance 95.3%～99.9%; During 40min, clearance 98%～100%.And when the processing time was increased to 40min, though energy consumption doubles, clearance had only risen 2.7%.Simultaneously, ∑ DDT, o during 20min, p'-DDE, p, p'-DDE, o, p'-DDD, p, p'-DDD, o, p'-DDT and p, p'-DDT concentration is respectively 9.23,5.36,3.39,0.048,0.023,0.29 and 0.13mgkg
-1, all be lower than place soil environment risk assessment screening value and place soil remediation suggestion desired value.Therefore from the angle of construction budget as can be known, 20min is the optimized processing time, can guarantee to reach repairing effect, also avoids too much energy waste simultaneously.When discharge power 1kW, processing time 20min, atmospherical discharges atmosphere, soil particle diameter 0～0.9mm, the clearance of DDTs is 95.3%～99.9%, has reached relevant criterion, can be used as the suitable condition of Low Temperature Plasma Treating DDTs contaminated soil.
Embodiment 5: adopt embodiment 3 equipment to investigate the processing time to the influence of polycyclic aromatic hydrocarbon (PAHs) clearance
For trying soil: pick up from jiangsu wuxi PAHs contaminated soil, its basic physical and chemical is: for examination soil basic physical and chemical be: water content 3.5%, organic 23.4gkg
-1, full nitrogen 1.44gkg
-1, full phosphorus 0.86gkg
-1, full potassium 12.3gkg
-1, cation exchange capacity 15.6cmolkg
-1Pollutant in soil mainly comprises 16 kinds of PAHs of EPA regulation, and soil passes through 4 orders successively behind natural air drying, 10 orders, and 20 purpose sub-sieves obtain respectively＜1mm, 1～2mm, 2～5mm soil particle.
Basic parameter arranges: discharge power 1kW, soil particle diameter＜1mm, atmospherical discharges atmosphere, frequency 50Hz and voltage 220V(standard line voltage); Processing time: establish a 10min and 15min2 level, each level is done 4 repetitions.Soil is crossed 60 mesh sieves after the low temperature plasma post processing, uses for analyzing PAHs content.
As shown in Figure 5, along with the increase in processing time, three rings of three kinds of different-grain diameters, Fourth Ring, five rings, six rings, total polycyclic aromatic hydrocarbon and benzo [a] pyrene concentration are remarkable downward trend.When the processing time was 15min, the clearance of total polycyclic aromatic hydrocarbon can reach 98.5%, and the clearance of benzo [a] pyrene is up to 99.9%.
Claims (9)
1. the apparatus for low-temperature plasma treatment of a soil persistent organic pollutant using, it is characterized in that comprising reactor and reaction bench, described reactor is made up of reactor container (1) and reactor cover plate (2), described reactor container is provided with air inlet (9) and gas outlet (10), and reactor cover plate (2) is located on the reactor container (1); Reaction bench comprises insulation board (7), conductive seat (13), low-temperature plasma electrical source (12) and fan (15), conductive seat (13) is provided with support bar (4), insulation board (7) is located on the support bar (4), insulation board (7) is provided with high-field electrode (6) and last binding post (11), conductive seat (13) is provided with earth electrode (3) and following binding post (14), high-field electrode (6) and earth electrode (3) are oppositely arranged, fan (15) is towards the electrode setting, last binding post (11) is connected with low-temperature plasma electrical source (12), following binding post (14) is connected with ground wire, and reactor is located between high-field electrode (6) and the earth electrode (3).
2. according to the apparatus for low-temperature plasma treatment of the described a kind of soil persistent organic pollutant using of claim 1, it is characterized in that described support bar (4) is provided with the insulation board arrangement for adjusting height, described arrangement for adjusting height is nut (5).
3. according to the apparatus for low-temperature plasma treatment of the described a kind of soil persistent organic pollutant using of claim 1, it is characterized in that two opposite flanks of described insulation board (7) are provided with adjusting nut (8), in order to the fixation reaction still.
4. according to the apparatus for low-temperature plasma treatment of the described a kind of soil persistent organic pollutant using of claim 1, it is characterized in that described high-field electrode (6) and earth electrode (3) are cylinder, the cylinder side is provided with one group of groove.
5. according to the apparatus for low-temperature plasma treatment of the described a kind of soil persistent organic pollutant using of claim 1, it is characterized in that described reactor is made up of quartz reaction kettle cover plate and reactor container, described reactor container is made of quartzy annulus and stainless steel base plate, offer two holes on the quartzy annulus, be connected with quartz ampoule on the hole.
6. according to the apparatus for low-temperature plasma treatment of the described a kind of soil persistent organic pollutant using of claim 1, it is characterized in that described low-temperature plasma electrical source power output is 0～2 kW, frequency-tuning range 5～30 kHz, the output voltage adjustable range is 0～30 kV.
7. the arbitrary described device of claim 1 ~ 6 is handled the method for soil persistent organic pollutant using, it is characterized in that step is: the first step, and the natural air drying contaminated soil after the screening is put into reactor, and make it evenly to cover the reactor bottom; Second step placed reactor between the electrode, and behind the connection power supply, dielectric barrier discharge produces low temperature plasma and the persistence organic pollutant reaction also makes it to remove.
8. handle the method for soil persistent organic pollutant using according to the described device of claim 7, it is characterized in that step is: when handling gesarex polluted soil, low-temperature plasma electrical source (12) power output 1 kW, processing times 20 min, atmospherical discharges atmosphere, soil particle diameter＜1 mm.
9. handle the method for soil persistent organic pollutant using according to the described device of claim 7, it is characterized in that step is: when handling polycyclic aromatic hydrocarbon pollution, low-temperature plasma electrical source (12) power output 1 kW, processing times 15 min, atmospherical discharges atmosphere, soil particle diameter＜1 mm.
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| CN104607447A (en) * | 2014-12-04 | 2015-05-13 | 江苏大学 | Organic polluted soil restoration method based on low temperature plasma technology and apparatus |
| CN104445528B (en) * | 2014-12-09 | 2016-06-22 | 南京大学 | A kind of device of homogeneous dielectric barrier discharge plasma for purification polluted-water |
| CN104445528A (en) * | 2014-12-09 | 2015-03-25 | 南京大学 | Device for purifying polluted water by using uniform dielectric barrier discharging plasma |
| CN104607457A (en) * | 2014-12-23 | 2015-05-13 | 中山大学 | Device for treating organic contaminated soil on plasma fluidized bed |
| CN104841689A (en) * | 2015-05-21 | 2015-08-19 | 浙江大学 | Method for degrading organic pollutant in soil by utilizing low-temperature plasmas |
| CN104907314B (en) * | 2015-05-27 | 2017-06-13 | 华中科技大学 | A kind of processing method of halo organic solid pollutant |
| CN104907314A (en) * | 2015-05-27 | 2015-09-16 | 华中科技大学 | Treating method for halogenated organic solid pollutants |
| CN106189379A (en) * | 2016-08-15 | 2016-12-07 | 宁波德泰化学有限公司 | A kind of white carbon black removes the method for PAHs |
| CN106734166A (en) * | 2016-12-23 | 2017-05-31 | 核工业西南物理研究院 | The device of Low Temperature Plasma Treating persistent organism contaminated soil |
| CN107597837A (en) * | 2017-10-24 | 2018-01-19 | 龙净科杰环保技术（上海）有限公司 | Flat low-temperature plasma soil remediation method and device |
| CN107617636A (en) * | 2017-10-24 | 2018-01-23 | 龙净科杰环保技术（上海）有限公司 | Screw type low-temperature plasma soil remediation method and device |
| CN109287058A (en) * | 2018-11-08 | 2019-01-29 | 南京农业大学 | A kind of cold sterilization core apparatus of high voltage electric field low temperature plasma |
| CN110252795A (en) * | 2019-05-08 | 2019-09-20 | 苏州维诗环境技术工程有限公司 | The apparatus for low-temperature plasma treatment and method of soil persistent organic pollutant |
| CN110913551A (en) * | 2019-11-29 | 2020-03-24 | 大连理工大学 | Device and method for generating uniform space plasma by atmospheric pressure dielectric barrier discharge |
| CN113477693A (en) * | 2021-07-09 | 2021-10-08 | 吉林大学 | In-situ electric heating desorption method for soil organic pollutants |
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