CN103272839B - 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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- CN103272839B CN103272839B CN201310157616.5A CN201310157616A CN103272839B CN 103272839 B CN103272839 B CN 103272839B CN 201310157616 A CN201310157616 A CN 201310157616A CN 103272839 B CN103272839 B CN 103272839B
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- 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
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.
Background technology
Persistence organic pollutant (Persistent Organic Pollutants is called for short POPs) is mainly divided into three major types: pesticide (drinox, Niran, DDT etc.), industrial chemical (Polychlorinated biphenyls and hexachloro-benzene) and the byproduct (dioxin and furans) in producing.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 easy enrichment of degraded, China's major part agricultural land soil and industrial land all can detect it and remain, and bring potential hazard to human security.Therefore, people are caused to pay close attention to widely.
POPs refer to by various surrounding medium (air, water, organism etc.) can long-distance migration long-term existence in environment, there is extended residual, bioconcentration, half volatile and high toxicity, human health and environment are had to the organic pollution materials of the natural of serious harm or Prof. Du Yucang.The phenomenons such as POP is by all means after entered environment, and can cause serious impact and destruction to the ecosystem, correlative study shows, organism is exposed to POPs and dysgenesia, deformity, organ also can be caused to increase, and body is dead.Harm is mainly contained: a class is the impact of the birth weight on children, the obstacle of skeleton development and the disorder of metabolism; Equations of The Second Kind is to nervous system, the disorder of notice, immune suppression; 3rd class is the harm to reproductive system.4th class is carcinogenic.Therefore, must carry out properly and science disposal the soil after persistence organic pollutant pollution, to ensure its safety.
At present, the recovery technique of conventional persistence organic pollutant mainly contains: the disposal of high temperature incineration, cement kiln, thermal desorption, mechanochemistry dehalogenation, vitrification etc., but high temperature incineration and cement kiln disposal technology require high, and there is the potential danger forming secondary pollution, thermal desorption, mechanochemistry dehalogenation and vitrification processing cost are higher.
In atmos low-temperature plasma technical gas discharge plasma, the nitrogen in electronics and air, oxygen, hydrone collide the high vibration excited state or electron excitation metastable state N that generate
2material, oxidizing species, these species act on pollutant, and final generation carbon dioxide and water, open new approach for removing noxious pollutant at low temperatures.Dielectric barrier discharge is a kind of mode producing low temperature plasma, it refers to a kind of nonequilibrium state gas discharge dielectric being inserted discharge space, when applying sufficiently high alternating voltage when between two electrodes, interelectrode gas can breakdown and produce electric discharge, namely create dielectric barrier discharge.
What patent JP2002153834 adopted is after pending soil is heated to uniform temperature, force the pollutant in pending soil to carry out the method for Low Temperature Plasma Treating after gas procedure effusion, the method is the original physicochemical property of obvious spoiled soil because of heating.What patent JP2004283684 adopted is method by carrying out Low Temperature Plasma Treating after volatile organic contaminant extracting in soil to dusty gas.But these two kinds of Measures compare are applicable to volatile organic contaminant contaminated soil and organic pollution pollutes time shorter soil, there is certain limitation for process persistence organic pollutant.And these two kinds for the treatment of system equipment investments are comparatively large, processing cost is higher.
Summary of the invention
The technical problem solved: the application, for severe persistent organism contaminated soil (especially contaminated soil of site), provides a kind of apparatus for low-temperature plasma treatment and the method with good repairing effect.
Technical scheme: a kind of apparatus for low-temperature plasma treatment of soil persistent organic pollutant, 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 reactor cover plate is located on 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 support bar, insulation board is provided with high-field electrode and upper binding post, and conductive seat is provided with earth electrode and lower binding post, and high-field electrode and earth electrode are oppositely arranged, fan is arranged towards electrode, upper binding post is connected with low-temperature plasma electrical source, and lower binding post is connected with ground wire, and reactor is located between high-field electrode and earth electrode.
Described support bar is provided with 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 fixation reaction still.
Described high-field electrode and earth electrode are cylinder, and cylindrical sides 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 up of quartzy annulus and stainless steel base plate, quartzy annulus offers two holes, hole is connected with quartz ampoule.
Described low-temperature plasma electrical source power output is 0 ~ 2kW, frequency-tuning range 5 ~ 30kHz, and output voltage adjustable range is 0 ~ 30kV.
The method of described device process soil persistent organic pollutant, step is: the first step, the natural air drying contaminated soil after screening is put into reactor, and makes it uniform fold bottom reactor; Second step, is placed in reactor between electrode, and after switching on power, dielectric barrier discharge produces low temperature plasma and persistence organic pollutant reacts and makes it to remove.
When processing gesarex polluted soil, low-temperature plasma electrical source power output 1kW, processing time 20min, atmospherical discharges atmosphere, soil particle diameter <1mm.
When processing 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 of the present invention and method, utilizes existing O in reactor
2, N
2collide with the high energy electron in the low temperature plasma that a small amount of water equimolecular and dielectric barrier discharge produce, generate 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, and remove pollutant efficiency high, equipment investment is little, and processing cost is low, is applicable to the small-scale test of persistency organic contaminant soil remediation.
Accompanying drawing explanation
Fig. 1 is the apparatus for low-temperature plasma treatment structural representation of soil persistent organic pollutant of the present invention;
Fig. 2 is reaction of low temperature plasma still structural representation in Fig. 1;
Fig. 3 is the impact of processing time on total DDT concentration;
Fig. 4 be the processing time to o, p'-DDE, p, p'-DDE, o, p'-DDT and p, the impact of p'-DDT concentration;
Fig. 5 is the processing time on the impact of total polycyclic aromatic hydrocarbon and benzo [a] pyrene concentration.
Reactor container 1 in 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, upper binding post 11, low-temperature plasma electrical source 12, conductive seat 13, lower binding post 14, fan 15.
Detailed description of the invention
Following examples further illustrate 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, the amendment do the inventive method, step or condition and replacement, all belong to scope of the present invention.
If do not specialize, the conventional means that technological means used in embodiment is well known to those skilled in the art.
Embodiment 1:
The Low Temperature Plasma Treating method of soil persistent organic pollutant of the present invention is mainly: the first step, natural air drying contaminated soil after screening is put into reactor, and make it uniform fold bottom reactor container 1, then reactor cover plate 2 is covered on reactor container 1; Second step, is placed on earth electrode 3 by reactor, regulate the height of high-field electrode 6 to make it to fit tightly with reactor by the nut 5 rotating stainless steel support bar 4, then the nut 8 tightening insulation board 7 both sides makes it to keep fixing; 3rd step, if need other electric discharge atmosphere of building besides air, can enter reaction system by required atmosphere by reactor air inlet 9, then discharge through gas outlet 10; 4th step, upper binding post 11 on the insulation board 7 of polytetrafluoroethylene (PTFE) material is connected with low-temperature plasma electrical source 12, lower binding post 14 on stainless steel conductive seat 13 is connected with ground wire, opens low-temperature plasma electrical source 12 and power output is set to 1kW, open cooling fan 15; 5th step, keeps good discharge condition, makes dielectric barrier discharge produce existing O in low temperature plasma and reaction system
2, N
2oH, H, O, O is generated with a small amount of water equimolecular
3, HO
2deng Active Radicals Produced, until these free radicals and contaminant molecule complete reaction, then regulating power is lower than closing low-temperature plasma electrical source 12 after 200W.
Embodiment 2:
A kind of apparatus for low-temperature plasma treatment of soil persistent organic pollutant, 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 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 support bar 4, insulation board 7 is provided with high-field electrode 6 and upper binding post 11, conductive seat 13 is provided with earth electrode 3 and lower binding post 14, high-field electrode 6 and earth electrode 3 are oppositely arranged, fan 15 is arranged towards electrode, upper binding post 11 is connected with low-temperature plasma electrical source 12, lower binding post 14 is connected with ground wire, and reactor is located between high-field electrode 6 and earth electrode 3.Described support bar 4 is provided with 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 fixation reaction still.Described high-field electrode 6 and earth electrode 3 are cylinder, and cylindrical sides 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 up of quartzy annulus and stainless steel base plate, quartzy annulus offers two holes, hole is connected with quartz ampoule.Low-temperature plasma electrical source (CTP-2000K, Nanjing Rong Man Electronics Co., Ltd.) power output is 0 ~ 2kW, and frequency-tuning range 5 ~ 30kHz, 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, comprises low-temperature plasma electrical source, two stainless steel discharge electrodes, reactor and external cooling fans.Described reactor is placed between two stainless steel electrodes, and three fits tightly.Described low-temperature plasma electrical source power output is 0 ~ 2kW, frequency-tuning range 5 ~ 30kHz, and output voltage adjustable range is 0 ~ 30kV.Described sparking electrode is the stainless steel cylinder of diameter 150mm, thickness 26mm, electrode sidewall periphery design 5 road grooves, and the surface area that this design adds electrode is beneficial to electrode heat radiation in discharge process.Described sparking electrode is made up of high-field electrode and earth electrode, the high-field electrode being wherein fixed on polytetrafluoroethylene (PTFE) material insulation board connects low-temperature plasma electrical source by positive pole, and the earth electrode being fixed on stainless steel base is connected with ground wire by negative terminal.Teflon insulation plate is supported on directly over stainless steel base by two threaded stainless steel columns.Reactor comprise a container and one piece of diameter be 214mm, thickness is the quartz cover plate of 3mm, this container by the tabular quartz annulus that a slice external diameter is 214mm, internal diameter is 150mm, thickness is 8mm and one piece of diameter be 168mm, thickness is that the stainless-steel sheet of 3mm is bonded up and down.In the quartzy annulus both sides of container, having a diameter is separately the aperture of 6mm, and this small pitch is from quartzy upper surface 1mm, and an external bending quartz round tube.This design can be used for the various gases passed in reactor needed for experimental design, thus builds Different hypothermia plasma discharge atmosphere.Described external cooling fan is NMB2110KL-03B-B65, power 3.6W, lowers the temperature for stainless steel electrode.
Embodiment 4: adopt embodiment 3 equipment to investigate the processing time to the impact of DDT (DDTs) clearance
For examination soil: pick up from Zhangjiakou DDT and discard production site, its basic physical and chemical is as shown in table 1.Pollutant in soil mainly comprises 6 kinds of DDT and derivatives etc. thereof, and soil, after natural air drying, crosses 20 orders (1mm) sieve, for subsequent use.
Table 1 is for the basic physical and chemical of examination soil
Basic parameter is arranged: 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 does 4 repetitions.After low temperature plasma post processing, soil crosses 60 mesh sieves, for analysis 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 declines comparatively slow; Between 15 ~ 20min, ∑ DDT is from 207.6mgkg
-1drop to 9.23mgkg
-1; After 20min, downward trend is mild.When being when treated 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 declines along with the increase in processing time, and o, p'-DDE concentration is then rise to some extent in the incipient stage, declines gradually after 5min.After 20min, each component downward trend all tends towards stability, and its concentration almost no longer changes.As seen from Figure 4, when the processing time is 20min, DDTs concentration sharply declines, and slightly declines afterwards, and clearance is 95.3% ~ 99.9%.
As shown in Table 2, when being when treated 20min, o, p'-DDD and p, the clearance of p'-DDD is 99.3% and 98.1%.
Table 2 processing time to o, p'-DDD and p, the impact of p'-DDD removal effect
Result shows, when processing time 5min, and o, p'-DDE concentration reaches maximum, and subsequently in significantly declining, 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, p'-DDT complete oxidation generates CO
2, HO
2deng, only there are part C-H key and C-Cl key fracture occurs thus generates o, p'-DDE.And p, p'-DDE concentration does not obviously first increase rear downward trend, also may be due to the p in soil, p'-DDT relative concentration be lower, the p of generation, and p'-DDE also lower thus variation tendency is not obvious.It is 20min, DDTs clearance 95.3% ~ 99.9% when treated; During 40min, clearance 98% ~ 100%.And when treated between when being increased to 40min, although energy consumption doubles, clearance only rises 2.7%.Meanwhile, ∑ 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 lower than place soil environmental risk assessment screening value and place soil remediation suggestion desired value.Therefore from the angle of construction budget, 20min is the optimized processing time, can ensure to reach repairing effect, also avoids too much energy waste simultaneously.As discharge power 1kW, processing time 20min, atmospherical discharges atmosphere, soil particle diameter 0 ~ 0.9mm, the clearance of DDTs is 95.3% ~ 99.9%, reaches 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 impact of polycyclic aromatic hydrocarbon (PAHs) clearance
For examination soil: pick up from jiangsu wuxi PAHs contaminated soil, its basic physical and chemical is: for examination physiochemical properties of soil 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
-1.Pollutant in soil mainly comprises 16 kinds of PAHs of EPA regulation, and soil is after natural air drying, and successively by 4 orders, 10 orders, 20 object sub-sieves, obtain <1mm, 1 ~ 2mm respectively, 2 ~ 5mm soil particle.
Basic parameter is arranged: discharge power 1kW, soil particle diameter <1mm, atmospherical discharges atmosphere, frequency 50Hz and voltage 220V(standard line voltage); In the processing time: establish 10min and 15min2 level, each level does 4 repetitions.After low temperature plasma post processing, soil crosses 60 mesh sieves, for analysis 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, always polycyclic aromatic hydrocarbon and benzo [a] pyrene concentration are remarkable downward trend.When being when treated 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 (3)
1. the apparatus for low-temperature plasma treatment of a soil persistent organic pollutant, 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 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 support bar (4), insulation board (7) is provided with high-field electrode (6) and upper binding post (11), conductive seat (13) is provided with earth electrode (3) and lower binding post (14), high-field electrode (6) and earth electrode (3) are oppositely arranged, fan (15) is arranged towards electrode, upper binding post (11) is connected with low-temperature plasma electrical source (12), lower binding post (14) is connected with ground wire, reactor is located between high-field electrode (6) and earth electrode (3), described support bar (4) is provided with 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 fixation reaction still, described high-field electrode (6) and earth electrode (3) are cylinder, and cylindrical sides 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 up of quartzy annulus and stainless steel base plate, quartzy annulus offers two holes, hole is connected with quartz ampoule.
2. the apparatus for low-temperature plasma treatment of a kind of soil persistent organic pollutant according to 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, output voltage adjustable range is 0 ~ 30 kV.
3. the method for device process soil persistent organic pollutant described in claim 1 or 2, is characterized in that step is: the first step, the natural air drying contaminated soil after screening is put into reactor, and makes it uniform fold bottom reactor; Second step, is placed in reactor between electrode, and after switching on power, dielectric barrier discharge produces low temperature plasma and persistence organic pollutant reacts and makes it to remove; Process gesarex polluted soil, low-temperature plasma electrical source (12) power output 1 kW, processing time 20 min, atmospherical discharges atmosphere, soil particle diameter <1 mm; Process polycyclic aromatic hydrocarbon pollution, low-temperature plasma electrical source (12) power output 1 kW, processing time 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 |
| 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 |
| CN106189379B (en) * | 2016-08-15 | 2018-11-30 | 宁波德泰化学有限公司 | A kind of method of carbon black removal 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 |
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| 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 |
| 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 |
| CN113477693B (en) * | 2021-07-09 | 2022-08-12 | 吉林大学 | In-situ electric heating desorption method for soil organic pollutants |
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