CN103752598A - Equipment and method for restoring heavy-metal-polluted soil by combination of leaching method and oxidation method - Google Patents
Equipment and method for restoring heavy-metal-polluted soil by combination of leaching method and oxidation method Download PDFInfo
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- CN103752598A CN103752598A CN201310749630.4A CN201310749630A CN103752598A CN 103752598 A CN103752598 A CN 103752598A CN 201310749630 A CN201310749630 A CN 201310749630A CN 103752598 A CN103752598 A CN 103752598A
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Abstract
The invention provides equipment for restoring heavy-metal-polluted soil by the combination of a leaching method and an oxidation method. The equipment comprises a leaching column, an oxidation tube, a first circulating pump and a second circulating pump, wherein the leaching column is internally provided with the polluted soil; a sieving mesh is arranged under the polluted soil, and a leaching nozzle is arranged above the polluted soil; the lower end of the leaching column is connected with a buffering groove, and the oxidation tube is connected with an absorbing tube; one end of the first circulating pump is connected with the buffering groove, and the other end of the first circulating pump is connected with the oxidation tube; one end of the second circulating pump is connected with the absorbing tube, and the other end of the second circulating pump is connected with a spraying tube. The equipment and the method provided by the invention have the advantages that since EDTA (Ethylene Diamine Tetraacetic Acid) is used as a leaching agent, heavy metal in the soil can be removed in a high-efficiency and fast manner, and the difficulties that the cost of the agent is large, the secondary pollution is caused and the subsequent treatment is relatively troublesome are overcome; by compounding of organic acid and a small amount of additive, the desorption and the solubilization of the heavy metal in the soil are enhanced, the application range of leaching liquid is expanded, a combined body of the leaching liquid and the heavy metal is easily absorbed for separation by an absorbing agent, and no secondary pollution to the environment is caused.
Description
Technical field
The present invention relates to a kind of Apparatus and method for of restoration of soil polluted by heavy metal, relate in particular to a kind of Apparatus and method for that utilizes drip washing co-oxidation method to carry out restoration of soil polluted by heavy metal.
Background technology
Along with causing containing in a large number the waste water of heavy metal, waste residue, developing rapidly of industry be discharged in soil by irrational in recent years.The soil of China's heavy metal pollution accounts for 1/6 left and right of total cultivated area, and annual contaminated by heavy metals grain is especially up to millions of tons.In part contaminated site, present the combined pollution features that coexist such as metal Cu, Pb, Zn, and pollution concentration is higher more.Due to features such as disguise, refractory organics and the irreversibilities of heavy metal, make heavy-metal contaminated soil not only large area cannot use, but also can jeopardize by the food chain relation between crops and the mankind mankind's life and health, also can directly have influence on function and the structure of soil ecosystem, finally biological and ecological is threatened safely, even jeopardize the health of human body.Because the mankind's activity also joins heavy metal in soil, make heavy-metal contaminated soil problem become more and more serious in addition.Therefore, the reparation of heavy-metal contaminated soil and improvement become environmental problem urgently to be resolved hurrily.
The improvement of the heavy-metal contaminated soil being applied in that at present both at home and abroad research relates to and actual process mainly contains solidifies and removes 2 kinds of approach.In recent years, around these two kinds of approach, different control measures and method have been developed, as solidified, reduction, agricultural regulation and control, biological prosthetic and phytoremediation etc., but these methods have not thorough, the consuming time length of processing, easily produce high malicious mesostate and the shortcoming such as be of limited application, thereby not yet in engineering, apply.In engineering, main method has following several at present: the method for improving the soil, electronic repairing method, heat treating process, sparkling technology and soil washing.Compared with soil washing, the method for improving the soil, electronic repairing method, heat treating process and vitrification there is secondary pollution or the scope of application little or expensive, all have comparatively obviously wait not enough.
Soil leaching is to use physics or chemical means that the organic and inorganic pollution in contaminated soil is carried out to process separate, that isolate, concentrate or carry out harmless treatment.Wherein drip washing medicament is the key component of drip washing, the eluent being in the news is in recent years divided into inorganic eluent (water, inorganic salts, inorganic acid etc.), organic eluent (citric acid, oxalic acid, malic acid etc.), chelating agent (EDTA, DTPA etc.) and surfactant (rhamnolipid, saponin etc.) etc.Washing expends large, the wasting of resources; Inorganic acid can cause the physicochemical property of soil to change, and makes soil present acidity; Although organic acid, to not too large harm of environment, just has effect for slight pollution soil, for high density pollution soil, can bring the problems such as drip washing reagent consumption is large, disposal cost is high; Surfactant output is lower, and production cost is high.
Based on the variety of problems of above-mentioned eluent, propose as eluent, to carry out drip washing contaminated soil with EDTA.EDTA can be combined with most of metal ion and be formed stable chelate, to the Cu in soil, Zn, Pb, Cd has higher removal efficiency, be widely used in the reparation of heavy-metal contaminated soil, but one of subject matter of EDTA washed off soil is chelating agent and heavy metal complex, be difficult to separate from extract.EDTA is a kind of poisonous medicament, and its complex compound is to be difficult to chemistry and biodegradation, therefore must before extracting, be removed, then by safe discharge.
Soil leaching technology be an application strong, can thoroughly remove the controlled and fireballing soil remediation improvement technology of pollutant, processing procedure, be usually used in the repairing and treating of contaminated site, in contaminated site reparation, be widely used abroad, and obtained good repairing effect.Wherein the selection of eluent is the key of recovery technique.The heavy metal eluent of having reported is mainly surfactant and acids eluent.Surfactant divides artificial synthetic complexing agent (EDTA etc.), biosurfactant (comprising rhamnolipid, sophorolipid, husky graceful and saponin of ancient India etc.).EDTA can be combined into stable chelate with most of metal ion because of it, to the Cu in soil, Zn, Pb, Hg, Cd and Cr etc. have higher removal efficiency, thereby are widely used in the reparation of heavy-metal contaminated soil, but EDTA exists the problems such as expensive, biological degradability is poor, recovery is difficult.In recent years, people start biosurfactant to replace EDTA for Soil leaching, but biosurfactant output is lower, and production cost is higher.Therefore, the plant-scale application of biosurfactant at present does not have advantage.Acids eluent mainly comprises inorganic acid solution (HC1 and HNO3 etc.), natural organic acids solution (citric acid, malic acid, oxalic acid, malonic acid, humic acid and fulvic acid etc.).Heavy metal in the maximized removal soil of inorganic acid energy, and cheap, but after drip washing, easily cause the physicochemical property of soil to change, make soil present acid, the soil of serious pollution that it is suitable for industrial waste.Natural organic acids has good removing ability to heavy metal, and acid gentle, biological degradability is good, and environment is not polluted, and is the environmentally friendly eluent that has very much application prospect.The research that adopts organic acid to carry out single type metallic pollution soil remediation has at present obtained certain result, and utilizes organic acid and the composite research with reparation multiple metal soil of additive combination and the also rarely seen report of processing of ring waste.Meanwhile, eluent loss of effective components is large, recovery time is long, reclaim concentrated pollutant is difficult to thorough elimination, easily causes pollutant entered environment system again, causes secondary pollution.
Summary of the invention
The problem to be solved in the present invention is to provide one can carry out oxidizing process restoration of soil polluted by heavy metal to ring waste, and the Apparatus and method for recycling.
For solving the problems of the technologies described above, the technical solution used in the present invention is: the equipment that a kind of drip washing co-oxidation method restoration of soil polluted by heavy metal is provided, comprise drip washing post, the in-built restoration of soil polluted by heavy metal that needs of described drip washing post, described heavy-metal contaminated soil to be repaired below is provided with screen cloth, its top is provided with drip washing shower nozzle, and drip washing shower nozzle connection one is used for supplementing the shower of leacheate, and described drip washing post lower end connects a dashpot by pipeline;
Oxidation tube, is filled with oxidant in described oxidation tube, and the liquid outlet of oxidation tube connects an adsorption tube, in described adsorption tube, is filled with adsorbent;
The first circulating pump, described the first pipeline of circulating pump one end and the lower end of dashpot are connected, and the pipeline of the other end is connected with the inlet of oxidation tube;
The second circulating pump, the pipeline of described second circulating pump one end is connected with adsorption tube, and the pipeline of the other end connects and is connected with shower.
Further, the inlet of described oxidation tube also connects an ozone generator.
Further, the periphery of described oxidation tube is provided with several uviol lamps.
Further, the pipeline between described dashpot and the first circulating pump is provided with a pressure regulator valve.
Further, described adsorbent is active carbon, tourmaline or flyash.
Utilize above-described equipment to carry out a method for drip washing co-oxidation method restoration of soil polluted by heavy metal, comprise the steps:
Waste liquid after step 3, drip washing, through oxidation, is separated heavy metal, and the waste liquid after drip washing is in the first circulating pump flows into oxidation tube, and the waste liquid after drip washing is by the oxidant oxidation in oxidized pipe;
Further, the organic acid in described step 1 is EDTA complexing agent, citric acid, malic acid, oxalic acid, malonic acid, humic acid or fulvic acid, and auxiliary agent is sodium chloride.
Further, the mass ratio of the organic acid in described step 1 and auxiliary agent is 5:1～2:1.
Further, the adsorbent in described step 4 is active carbon, tourmaline or flyash.
Further, the waste liquid after oxidation in described step 4 and the liquid-solid ratio of adsorbent are 20:1～5:1.
Advantage and good effect that the present invention has are: use EDTA can efficiently and fast remove the heavy metal in soil as eluent; Simultaneously, utilize the method for ozone/ultra-violet radiation to process leacheate, not only solve EDTA and produced secondary pollution as leacheate, and shortcoming that can not biology/chemical degradation, remove in time the heavy metal in leacheate, and can recycle residual waste solution, can save a large amount of EDTA and water resource; The method of ozone/ultra-violet radiation and EDTA drip washing earth pillar is combined, and the method reagent cost that has overcome existing EDTA drip washing heavy-metal contaminated soil is large, produces secondary pollution, the difficult problem that subsequent treatment is cumbersome; By organic acid and a small amount of additive compound, promote the desorb solubilising of heavy metal in soil, widened the scope of application of leacheate, the combination of leacheate and heavy metal is easy to by adsorbent adsorbing separation, and environment is not caused to secondary pollution, the spread that is especially applicable to moderate heavy-metal contaminated soil is used; Have high to heavy metal removing rate, leacheate can reuse, take into account the factors such as environment friendly and low cost.
Accompanying drawing explanation
Fig. 1 is the schematic diagram of the specific embodiment of the equipment of drip washing co-oxidation method restoration of soil polluted by heavy metal of the present invention.
In figure:
1. drip washing post, 2. screen cloth, 3. dashpot, 4. pressure regulator valve, 5. the first circulating pump,
6. ozone generator, 7. oxidation tube, 8. uviol lamp, 9. adsorption tube, 10. the second circulating pump,
11. contaminated soils, 12. drip washing shower nozzles.
The specific embodiment
For to the more deep understanding of the present invention, enumerate a specific embodiment below, and by reference to the accompanying drawings, the present invention is described in further detail.
In the present embodiment, as shown in Figure 1, the equipment of drip washing co-oxidation method restoration of soil polluted by heavy metal comprises drip washing post 1, dashpot 3, oxidation tube 7, adsorption tube 9, the first circulating pump 5 and the second circulating pump 10; Contaminated soil 11 is housed in drip washing post 1, and contaminated soil 11 belows are provided with screen cloth 2, and its top is provided with drip washing shower nozzle 12, and drip washing shower nozzle 12 connects a shower that is used for supplementing leacheate, and drip washing post lower end connects dashpot 3 by pipeline; In oxidation tube 7, be filled with oxidant, the inlet of oxidation tube 7 also connects an ozone generator 6, and the liquid outlet of oxidation tube 7 connects adsorption tube 9, in adsorption tube 9, is filled with adsorbent, and the periphery of oxidation tube 7 is provided with several uviol lamps 8; The pipeline of first circulating pump 5 one end is connected with the lower end of dashpot 4, and the pipeline of the other end is connected with the inlet of oxidation tube 7; The pipeline of second circulating pump 10 one end is connected with adsorption tube 9, and the pipeline of the other end connects and is connected with shower, and the pipeline between dashpot 3 and the first circulating pump 5 is provided with a pressure regulator valve 4; In the present embodiment, adsorbent is active carbon (tourmaline or flyash).
Utilize above-described equipment to carry out a method for drip washing co-oxidation method restoration of soil polluted by heavy metal, comprise the steps:
Waste liquid after step 3, drip washing, through oxidation, is separated heavy metal, and the waste liquid after drip washing is in the first circulating pump flows into oxidation tube, and the waste liquid after drip washing is by the oxidant oxidation in oxidized pipe;
Organic acid in step 1 is EDTA complexing agent, citric acid, malic acid, oxalic acid, malonic acid, humic acid or fulvic acid, and auxiliary agent is sodium chloride, and the mass ratio of organic acid and auxiliary agent is 5:1～2:1; The waste liquid after oxidation in step 4 and the liquid-solid ratio of adsorbent are 20:1～5:1.
The operation principle of the equipment of restoration of soil polluted by heavy metal in the present embodiment: eluent carries out drip washing by drip washing post to soil, after drip washing, produce the waste liquid containing heavy metal complex, by the complex compound of ozone/ultra-violet radiation oxidation Decomposition heavy metal in waste liquid, heavy metal after decomposition is adsorbed the Activated Carbon Adsorption Separation in device, and remaining waste liquid is transported in drip washing post and is recycled as eluent by the second circulating pump.
Wherein, ozone is divided into two steps for the oxidation of organic compound: use ozone molecule direct oxidation or rely on the hydroxyl radical free radical producing.Under normal oxidation condition, the concentration of hydroxyl radical free radical is very little, is exactly the oxidation that relies on ozone substantially, because of hydroxyl radical free radical oxidability in solution very strong, so use ultra-violet radiation, can promote like this formation of hydroxyl radical free radical, its concentration is raise, in oxidation in the highest flight.A closed-circuit system of this equipment composition is divided into two steps and processes leacheate: the first step is to use leacheate drip washing to be subject to the soil of heavy metal pollution; Second step is to use hydroxyl radical free radical that the solution containing heavy metal complex is decomposed, and then by active carbon, carrys out adsorbent solution, and the solution after absorption is directly delivered to drip washing post top by pipeline and the second circulating pump, to recycle residue leacheate.
It is as follows respectively to the soil charging drip washing situation of heavy metal pollution that the present embodiment is enumerated four kinds of leacheates:
The first leacheate: using EDTA as eluent, be that EDTA eluent carries out drip washing by drip washing post to soil, after drip washing, produce the waste liquid containing EDTA-heavy metal complex, by the complex compound of EDTA-heavy metal in ozone/ultra-violet radiation oxidation Decomposition waste liquid, heavy metal after decomposition is adsorbed the Activated Carbon Adsorption Separation in device, residue recycles as eluent by circulation pumping drip washing post containing the waste liquid of EDTA, has saved a large amount of water resources.
The second leacheate: the lead-contaminated soil of 5g is put in 250ml conical flask, adopt the eluent (both mass ratioes are 2:1) of citric acid and sodium chloride mixture, the liquid-solid ratio of eluent and soil is 20:1, then place it in and on magnetic stirring apparatus, stir 2h, with pipette, respectively the supernatant after stirring is taken out to about 4ml afterwards and put into clean centrifuge tube, centrifuge is set to rotating speed 5000r/min, centrifugal 10 minutes, carries out Separation of Solid and Liquid.Take out again and filter, dilute, with Atomic Absorption Spectrometer, measure the concentration of heavy metal in solution.By remaining soil in conical flask, use vavuum pump suction filtration, air-dry rear with scales/electronic balance weighing, micro-wave digestion, by the concentration of heavy metal in Atomic Absorption Spectrometer measurement pedotheque simultaneously.Record clearance plumbous after drip washing and reach 56.1%, the removal efficiency (44.9%) of lead when citric acid is as eluent separately.In waste liquid after drip washing, by liquid-solid ratio 20:1, put into active carbon, after charcoal absorption, in waste liquid, 93.5% lead is removed.
The third leacheate: the cadmium pollution soil of 5g is put in 250ml conical flask, adopt the eluent (both mass ratioes are 4:1) of oxalic acid and sodium chloride mixture, the liquid-solid ratio of eluent and soil is 20:1, then place it in and on magnetic stirring apparatus, stir 2h, with pipette, respectively the supernatant after stirring is taken out to about 4ml afterwards and put into clean centrifuge tube, centrifuge is set to rotating speed 5000r/min, centrifugal 10 minutes, carries out Separation of Solid and Liquid.Take out again and filter, dilute, with Atomic Absorption Spectrometer, measure the concentration of heavy metal in solution.By remaining soil in conical flask, use vavuum pump suction filtration, air-dry rear with scales/electronic balance weighing, micro-wave digestion, by the concentration of heavy metal in Atomic Absorption Spectrometer measurement pedotheque simultaneously.Record clearance plumbous after drip washing and reach 91.2%, the removal efficiency (60.7%) of cadmium when citric acid is as eluent separately.In waste liquid after drip washing, by liquid-solid ratio 10:1, put into tourmaline powder, after tourmaline powder absorption, in waste liquid, 87.7% cadmium is removed.
The 4th kind of leacheate: the cadmium pollution soil of 5g is put in 250ml conical flask, adopt the eluent (both mass ratioes are 5:1) of citric acid and sodium chloride mixture, the liquid-solid ratio of eluent and soil is 20:1, then place it in and on magnetic stirring apparatus, stir 2h, with pipette, respectively the supernatant after stirring is taken out to about 4ml afterwards and put into clean centrifuge tube, centrifuge is set to rotating speed 5000r/min, centrifugal 10 minutes, carries out Separation of Solid and Liquid.Take out again and filter, dilute, with Atomic Absorption Spectrometer, measure the concentration of heavy metal in solution.By remaining soil in conical flask, use vavuum pump suction filtration, air-dry rear with scales/electronic balance weighing, micro-wave digestion, by the concentration of heavy metal in Atomic Absorption Spectrometer measurement pedotheque simultaneously.Record clearance plumbous after drip washing and reach 94.3%, the removal efficiency (60.7%) of cadmium when citric acid is as eluent separately.In waste liquid after drip washing, by liquid-solid ratio 5:1, put into flyash, after Powder ash adsorption, in waste liquid, 84.4% cadmium is removed.
Above embodiments of the invention are had been described in detail, but described content is only preferred embodiment of the present invention, can not be considered to for limiting practical range of the present invention.All equalization variations of doing according to the scope of the invention and improvement etc., within all should still belonging to this patent covering scope.
Claims (10)
1. the equipment of a drip washing co-oxidation method restoration of soil polluted by heavy metal, it is characterized in that: comprise drip washing post, the in-built restoration of soil polluted by heavy metal that needs of described drip washing post, described heavy-metal contaminated soil to be repaired below is provided with screen cloth, its top is provided with drip washing shower nozzle, drip washing shower nozzle connection one is used for supplementing the shower of leacheate, and described drip washing post lower end connects a dashpot by pipeline;
Oxidation tube, is filled with oxidant in described oxidation tube, and the liquid outlet of oxidation tube connects an adsorption tube, in described adsorption tube, is filled with adsorbent;
The first circulating pump, described the first pipeline of circulating pump one end and the lower end of dashpot are connected, and the pipeline of the other end is connected with the inlet of oxidation tube;
The second circulating pump, the pipeline of described second circulating pump one end is connected with adsorption tube, and the pipeline of the other end connects and is connected with shower.
2. the equipment of drip washing co-oxidation method restoration of soil polluted by heavy metal according to claim 1, is characterized in that: the inlet of described oxidation tube also connects an ozone generator.
3. the equipment of drip washing co-oxidation method restoration of soil polluted by heavy metal according to claim 1, is characterized in that: the periphery of described oxidation tube is provided with several uviol lamps.
4. the equipment of drip washing co-oxidation method restoration of soil polluted by heavy metal according to claim 1, is characterized in that: the pipeline between described dashpot and the first circulating pump is provided with a pressure regulator valve.
5. the equipment of drip washing co-oxidation method restoration of soil polluted by heavy metal according to claim 1, is characterized in that: described adsorbent is active carbon, tourmaline or flyash.
6. utilize equipment according to claim 1 to carry out a method for drip washing co-oxidation method restoration of soil polluted by heavy metal, comprise the steps:
Step 1, configuration leacheate, configure EDTA or organic acid become to leacheate with additive compound;
Step 2, leacheate is immersed to heavy-metal contaminated soil to be repaired, leacheate evenly sprays in the heavy-metal contaminated soil to be repaired in drip washing post by shower, drip washing shower nozzle;
Waste liquid after step 3, drip washing, through oxidation, is separated heavy metal, and the waste liquid after drip washing is in the first circulating pump flows into oxidation tube, and the waste liquid after drip washing is by the oxidant oxidation in oxidized pipe;
Step 4, after oxidation, waste liquid is by adsorbent by heavy metal adsorption wherein, and the waste liquid after oxidation passes in adsorption tube, and adsorbent will absorption long heavy metal of waste liquid after oxidation in adsorption tube;
Step 5, the residual waste solution after having adsorbed heavy metal will recycle as leacheate, and the second circulating pump imports the residual waste solution after having adsorbed heavy metal in the shower of drip washing post top, continues to treat restoration of soil polluted by heavy metal and carries out drip washing.
7. the method for drip washing co-oxidation method restoration of soil polluted by heavy metal according to claim 6, it is characterized in that: the organic acid in described step 1 is EDTA complexing agent, citric acid, malic acid, oxalic acid, malonic acid, humic acid or fulvic acid, auxiliary agent is sodium chloride.
8. the method for drip washing co-oxidation method restoration of soil polluted by heavy metal according to claim 6, is characterized in that: the organic acid in described step 1 and the mass ratio of auxiliary agent are 5:1～2:1.
9. the method for drip washing co-oxidation method restoration of soil polluted by heavy metal according to claim 6, is characterized in that: the adsorbent in described step 4 is active carbon, tourmaline or flyash.
10. the method for drip washing co-oxidation method restoration of soil polluted by heavy metal according to claim 6, is characterized in that: the waste liquid after oxidation in described step 4 and the liquid-solid ratio of adsorbent are 20:1～5:1.
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