CN101648207B - Chemical oxidation remediation method for organism-contaminated soil and remediation device - Google Patents
Chemical oxidation remediation method for organism-contaminated soil and remediation device Download PDFInfo
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- CN101648207B CN101648207B CN200910091596XA CN200910091596A CN101648207B CN 101648207 B CN101648207 B CN 101648207B CN 200910091596X A CN200910091596X A CN 200910091596XA CN 200910091596 A CN200910091596 A CN 200910091596A CN 101648207 B CN101648207 B CN 101648207B
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Abstract
The invention relates to a chemical oxidation remediation method for organism-contaminated soil and a remediation device. The device comprises an oxidant pot, a catalyst pot, a chelating agent pot, a flexible pipe, an electric valve, a control apparatus, a valve switch, a pump, a flow valve, a reactor, a stirrer, a stirrer switch, a sealing cover, a liquid inlet pipe, an exhaust pipe, a gas-liquid separating apparatus and a tail gas treating apparatus. The method comprises the following steps: placing contaminated soil into the reactor; firstly injecting 0.03-0.4mol/(kg soil) of citric acid into the reactor through the chelating agent pot; then adding 0-0.4mol/(kg soil) of catalyst ferrous sulfate in the catalyst pot, and adding water to be dissolved to prepare 0.5mol/L of catalyst; injecting the catalyst into the reactor by the pump; pumping 1-2mol/(kg soil) of oxidant hydrogen peroxide into the reactor; and fully stirring the three preparations and the contaminated soil by the stirrer in the reactor to oxidize and degrade polycyclic aromatic hydrocarbon in the soil, and the removal rate of pollutants in the soil exceeds 80 percent. The invention has high efficiency on organics-contaminated soil remediation and can not cause secondary pollution to the soil.
Description
Technical field
The present invention relates to a kind of chemical oxidation restorative procedure and equipment of organic polluted soil, belong to field of environment engineering technology, the processing of solid dielectrics such as multiclass organic polluted soil such as the polycyclic aromatic hydrocarbon that can be applied in industries such as chemical industry, petroleum industry, to produce, benzene series thing, petroleum hydrocarbon, organic agricultural chemicals, organic solvent.
Background technology
Along with developing rapidly of chemical industry, increasing organic pollution enters into soil and groundwater environment, be difficult to can be remained in the environment for a long time by biodegradable pollutant, and the conversion that moves about, bring great hidden danger.Especially some chemical plant, the leakage of a large amount of organic pollutions that cause owing to reasons such as leakages causes organic pollution very high concentrations in soil and the underground water.The constantly migration and transforming of these pollutants enters human body by respiratory tract, alimentary canal etc., and human body is formed great threat, a lot of organic pollutions, and for example polycyclic aromatic hydrocarbon etc. all has chemical carcinogenesis and photic toxic effect.
Reparation at organic polluted soil has physical method, comprises excavating landfill method, ventilation method etc.; Biological method comprises and throws bacterium method, bioventing process etc.; Chemical method comprises burning method, chemical cleaning method, photochemical degradating method, chemistry redox method etc.Bigger at contaminated area, the situation that pollutant levels are high, the quantities that adopts physical method to expend is big, cost is also corresponding higher, the biological method required time is longer, be difficult at short notice pollutant effectively be removed, and chemical method is than the two kinds of methods in front, have its remarkable advantages, comprise insensitive to pollutant kind, be swift in response, remediation efficiency height and rehabilitation cost be lower or the like.
Many laboratory experiments have all been studied the detergent power of chemical oxidizing agent for organic polluted soil, and oxidant commonly used comprises hydrogen peroxide, potassium permanganate, sodium peroxydisulfate etc.Hydrogen peroxide very easily decomposes under alkali condition, and service efficiency is not high separately, the researcher is arranged by adding ferrous sulfate, and catalyzing hydrogen peroxide decomposes the generation hydroxy radical, thus the oxidation organic pollution.But because very easily oxidation of ferrous ion, when causing it to be applied in the in-situ chemical oxidation reparation, often efficient is not high, and ferrous ion very easily forms precipitation under condition of neutral pH.Therefore, need to add suitable assistant, the pH that keeps oxidant and pollutant reaction as much as possible is near 3, suppress the decomposition of hydrogen peroxide, and guarantee that ferrous ion does not form precipitation, it is not oxidized to control ferrous ion simultaneously, could guarantee higher oxidation efficiency.
At present, processing for some organic polluting waters, many comparatively ripe method and apparatus have been arranged, steam treatment for the high concentration organic polluted soil, also the someone has developed special device, but organic polluted soil is taked the chemical oxidation treatment mode, at present the domestic equipment that does not still have independent research.
Summary of the invention
Technology of the present invention is dealt with problems: when utilizing hydrogen peroxide and ferrous ion oxidation organic polluted soil, hydrogen peroxide very easily decomposes, and the easy oxidation of ferrous ion reaches problems such as precipitation can take place under neutrallty condition, by adding the acid chelating agent citric acid, guarantee pH near 3 on the one hand, suppress the decomposition of hydrogen peroxide, and make ferrous ion not form precipitation, and form chelate with ferrous ion, and slowly discharge ferrous ion, improve the removal efficient of oxidant to pollutant.
Simultaneously, independent research chemical oxidation prosthetic appliance is handled the high concentration organic polluted soil.
The present invention relates to restorative procedure shown below and equipment:
The step of the chemical oxidation restorative procedure of organic polluted soil is:
A) citric acid with 0～0.4mol/ (kg soil) dissolves in the chelating agent jar;
B) simultaneously the ferrous sulfate of 0.03～0.4mol/ (kg soil) is added in the catalyst tank, be dissolved in water, be configured to the catalyst of 0.5mol/L;
C) simultaneously the hydrogenperoxide steam generator of 1～2mol/ (kg soil) is added in the oxidant jar;
D) organic polluted soil is inserted reactor, agitating device is arranged at the reactor vessel bottom;
E) earlier with the citric acid solution in the chelating agent jar in (A) step, be injected in the reactor vessel; With the catalyst in the catalyst tank in (B) step, go in the reactor vessel again by infusion;
F) simultaneously with in the slow injecting reactor container of hydrogenperoxide steam generator in the oxidant jar in (C) step;
G) treat (E), (F) in the step three kinds of preparations in the reactor after, stirred 0.5～2 hour with agitating device, preparation fully mixed with contaminated soil and react;
H) after escaping gas separates by gas-liquid separation device in the course of reaction, utilize organic solvent-normal hexane to absorb.
A kind of equipment of realizing above-mentioned restorative procedure, it comprises oxidant jar 1, catalyst tank 2, chelating agent jar 3, flexible pipe 4, electrically operated valve 5, control device 6, valve switch 7, pump 8, flow valve 9, reactor 10, agitator 11, whip switch 12, seal cover 13, feed tube 14, blast pipe 15, gas-liquid separation device 16, exhaust gas processing device 17 compositions; Wherein, oxidant jar 1, catalyst tank 2 and chelating agent jar 3 all are connected to control device 6 by flexible pipe 4, and the switch 7 on the control device is used to control electrically operated valve 5 and flow; Electrically operated valve 5 is the flexible pipe closure of control connection oxidant jar 1, catalyst tank 2 or chelating agent jar 3 respectively; Pump 8 and reactor 10 are connected with flexible pipe, built-in agitator 11 in the reactor 10, and there is seal cover 13 on the top, and is connected with feed tube 14 and blast pipe 15; Agitator 11 is a roller type, and the switch 12 on next door is used to control the operation of agitator; Reactor 10 is connected with gas-liquid separation device 16 by blast pipe 15, is connected with exhaust gas processing device 17 by blast pipe again.
During work, in reactor 10 containers organic polluted soil is arranged; By control device 6 flexible pipe 4 is opened, by pump 8 with in three kinds of preparation injecting reactor 10 containers, stir by agitator 11, three kinds of preparations are fully mixed with organic polluted soil, the gas that the reaction back produces is absorbed by the n-hexane in the exhaust gas processing device 17 after separating by gas-liquid separation device 16.
The present invention's advantage compared with prior art is:
(1) owing to keep pH at acid condition, the decomposition of hydrogen peroxide is controlled, and ferrous ion can not form precipitation, also can oxidized formation iron ion;
(2) mode that adopt to stir, accelerating oxidation agent and contaminated soil contacts effectively;
(3) have for the organic pollution in the high density pollution soil and remove effect preferably, oxidable pollutant comprises: polycyclic aromatic hydrocarbon, benzene series thing, petroleum hydrocarbon, organic agricultural chemicals, chloro-carbon solvents such as trichloro-ethylene, tetrachloro-ethylene;
(4) whole device is all airtight in course of reaction, and therefore design exhaust gas processing device in reaction rear end can not cause the dissipation of gaseous organic pollutant, can effectively avoid secondary pollution.
Description of drawings
Fig. 1 is the chemical oxidation restorative procedure and device schematic diagram of organic material contaminated soil of the present invention.
The specific embodiment
Utilize equipment of the present invention, the contaminated soil that will handle adds in the reactor 10, cover seal cover 13, the chelating agent citric acid adding of 0～0.4mol/ (kg soil) is equipped with in the chelating agent jar 3 of a certain amount of deionized water, open the switch of controlling on the control device 6 with the tank connected electrically operated valve 5 of catalyst 7, utilize pump 8 to extract, earlier after in flexible pipe 4 and feed tube 14 injecting reactors 10; Then with the ferrous solution that in catalyst tank 2, is configured to 0.5mol/L of catalyst sulfuric acid of 0.03～0.4mol/ (kg soil), adopting uses the same method is added in the reactor 10, open the switch 12 of agitator 11 when annotating, stir, make ferrous ion and chelating agent generation chelation, guarantee that ferrous ion is not oxidized and form precipitation of hydroxide; At last, the oxidants hydrogen peroxide of 1～2mol/ in the oxidant jar 1 (kg soil) used the same method to be pumped in the reactor 10, utilizes agitating device to stir, and preparation for repairing and soil fully are mixed and react, thereby effectively with the organic pollution oxidation removal.The waste gas that produces in the reaction is absorbed by the n-hexane in the exhaust gas processing device 17 after entering gas-liquid separation device 16 and separate by blast pipe.
Method and apparatus of the present invention, not only the original position reparation for organic polluted soil has directive significance, and can be used for the dystopy processing of organic polluted soil or solid waste.Equipment has designed exhaust gas processing device, and the gaseous organic pollutant of overflowing during with reaction feeds in the organic solvent, prevents its dissipation, causes secondary pollution.
Method of the present invention comprises:
Add the acid chelating agent citric acid according to certain operation in reactor, addition is 0～0.4mol/ (a kg soil); It is ferrous to add catalyst sulfuric acid according to certain operation then, and the addition of catalyst is 0～0.3mol/ (a kg soil); Add oxidants hydrogen peroxide at last, addition is 1～2mol/kg soil.
Chelating agent adds operation:
In order to reduce Fe
2+Oxidation, by adding chelating agent, form chelate, thereby discharge Fe lentamente
2+, and add acid chelating agent when realizing this purpose, can also partly suppress the decomposition of hydrogen peroxide, and Fe
2+Precipitation.Therefore select for use citric acid as chelating agent, add after being dissolved in ionized water.
The chelating agent adding method is: in the chelating agent jar that deionized water is housed, it is fully dissolved a certain amount of citric acid, by pump it is imported in the reaction system then, mix with contaminated soil, stir by agitator and form mud.
Catalyst adds operation:
Proof is not being added catalyst and is being added under two kinds of situations of catalyst by experiment, and oxidants hydrogen peroxide is very big for the oxidation efficiency difference of target contaminant, thinks the interpolation catalyst Fe
2+Can generate hydroxyl free radical with hydroperoxidation, hydroxyl free radical has strong oxidizing property, and its oxidation-reduction potential is more much bigger than hydrogen peroxide, can be effectively with the organic pollution oxidation removal in the soil.Fe
2+Can be by adding ferrous sulfate, frerrous chloride and obtaining.
The catalyst adding method is: take by weighing a certain amount of ferrous sulfate in catalyst tank, add deionized water dissolving, be configured to the solution of 0.5mol/L, utilize pump to be injected in the oxidative system then, by the agitator stirring it is fully mixed with the chelating agent citric acid that adds earlier, reaction generates chelating ferrous ion, avoids oxidation or forms precipitation.
Specific embodiment
Be embodiments of the invention below
The engineering lab scale is provided with 5 case study on implementation, and 2 comparison cases are specifically handled as table 1.Utilize the equipment repairing polluted soil concrete steps of independent research as follows: in reactor, to add natural pollution soil 20kg to be repaired.With 0,0.2,0.3 or the chelating agent citric acid of 0.4mol/ (kg soil) be dissolved in the deionized water, add in the reactor, utilize agitator to stir; With 0.03,0.2,0.3 or the ferrous solution that is configured to of catalyst sulfuric acid of 0.4mol/ (kg soil), utilize pump to be added in the reactor then, form chelate with the citric acid that adds earlier, and pH is dropped to about 2～3; The oxidants hydrogen peroxide that adds 1～2mol/ (kg soil) at last.Reactor is tight with the seal cover lid, is connected with blast pipe on the reactor, and the reaction escaping gas is accepted in the exhaust gas processing device on next door, is added with n-hexane in this device, can effectively prevent the dissipation of gas pollutant, avoids environment is caused secondary pollution.After oxidant adds, utilize agitator to stir 0.5～2 hour, oxidant and soil are fully mixed, and fully reaction.Afterwards, leave standstill sampling and measuring pollutant levels after 24 hours.
Table 1 engineering lab scale is handled change in concentration and the clearance of P in soil AHs
Method of the present invention is added acid chelating agent and is kept being reflected under the acid condition carrying out, and suppresses the decomposition of hydrogen peroxide, reduces Fe
2+Oxidation and precipitation, slowly discharge Fe
2+,, reach the purpose of repairing polluted soil with hydroperoxidation generation free radical, the organic pollution of the efficient oxidation soil middle and high concentration.Embodiment 1 and 2 presentation of results add H
2O
2And ferrous sulfate, but do not add chelating agent, make PAHs in the soil descend 85 and 26mg/kg respectively, clearance is compared with comparative example and has been improved 8.6% and 65.8%.In embodiment 3,4 and 5, three kinds of chemicals increase consumption gradually according to 5: 1: 1 ratio, and the clearance of PAHs reaches 80.1% with embodiment 4 maximums, and three embodiment are all than comparative example height.The application of this explanation patent preparation for repairing prescription of the present invention can effectively improve the removal ability of pollutant in soil.At comparative example 2, promptly only add the processing that water does not use preparation for repairing, than raising to some extent before the reaction, this is to stir because only add deionized water to the concentration of reaction back PAHs on the contrary, some PAHs that are adsorbed in the soil particle are desorbed, the concentration of PAHs is raise.
Claims (3)
1. the chemical oxidation restorative procedure of an organic material contaminated soil is characterized in that step is:
(1) dissolves in the citric acid chelating agent jar with 0.2～0.4mol/kg organic matter pollution soil;
(2) ferrous sulfate is added in the catalyst tank, it is 0.03～0.4mol that every kilogram of organic matter pollutes the ferrous amount of soil adding solid sulphuric acid, and water filling is dissolved, and is configured to the catalyst of 0.5mol/L;
(3) simultaneously 1～2mol/kg organic matter is polluted in the hydrogenperoxide steam generator adding oxidant jar of soil;
(4) organic material contaminated soil is inserted reactor, agitating device is arranged at the reactor vessel bottom;
(5) earlier with the citric acid solution in the chelating agent jar in (1) step, be injected in the reactor vessel; With the catalyst in the catalyst tank in (2) step, go in the reactor vessel again by infusion;
(6) then with in the slow injecting reactor container of hydrogenperoxide steam generator in the oxidant jar in (3) step;
(7) treat (5), (6) in the step three kinds of preparations in the reactor after, stirred 0.5～2 hour with agitating device, preparation fully mixed with contaminated soil and react;
(8) after escaping gas separates by gas-liquid separation device in the course of reaction, utilize organic solvent-normal hexane to absorb.
2. a realization is according to the equipment of the described restorative procedure of claim 1, it is characterized in that: comprise oxidant jar (1), catalyst tank (2), chelating agent jar (3), flexible pipe (4), electrically operated valve (5), control device (6), valve switch (7), pump (8), flow valve (9), reactor (10), agitator (11), whip switch (12), seal cover (13), feed tube (14), blast pipe (15), gas-liquid separation device (16), exhaust gas processing device (17) is formed, wherein, oxidant jar (1), catalyst tank (2) and chelating agent jar (3) all are connected to control device (6) by flexible pipe (4), and the valve switch on the control device (7) is used to control electrically operated valve (5) and flow; Electrically operated valve (5) is the flexible pipe closure of control connection oxidant jar (1), catalyst tank (2) or chelating agent jar (3) respectively; Pump (8) is connected with flexible pipe with reactor (10), built-in agitator (11) in the reactor (10), and there is seal cover (13) on the top, and is connected with feed tube (14) and blast pipe (15); Reactor (10) is connected with gas-liquid separation device (16) by blast pipe (15), is connected with exhaust gas processing device (17) by blast pipe again.
3. equipment according to claim 2 is characterized in that: described agitator (11) is a roller type, and the whip switch on next door (12) is used to control the operation of agitator.
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| CN200910091596XA CN101648207B (en) | 2009-08-28 | 2009-08-28 | Chemical oxidation remediation method for organism-contaminated soil and remediation device |
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| CN200910091596XA CN101648207B (en) | 2009-08-28 | 2009-08-28 | Chemical oxidation remediation method for organism-contaminated soil and remediation device |
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| CN101648207B true CN101648207B (en) | 2011-04-06 |
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