CN108213064A - A kind of medicament of in-situ immobilization high concentration polycyclic aromatic hydrocarbon pollution and its application - Google Patents
A kind of medicament of in-situ immobilization high concentration polycyclic aromatic hydrocarbon pollution and its application Download PDFInfo
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- CN108213064A CN108213064A CN201711267906.XA CN201711267906A CN108213064A CN 108213064 A CN108213064 A CN 108213064A CN 201711267906 A CN201711267906 A CN 201711267906A CN 108213064 A CN108213064 A CN 108213064A
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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
- B09C1/08—Reclamation of contaminated soil chemically
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K17/00—Soil-conditioning materials or soil-stabilising materials
- C09K17/02—Soil-conditioning materials or soil-stabilising materials containing inorganic compounds only
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C2101/00—In situ
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Abstract
A kind of medicament of in-situ immobilization high concentration polycyclic aromatic hydrocarbon pollution and its application, active ingredient is micro-nano iron plate and sodium peroxydisulfate, the present invention generates the free radical of strong oxidizing property using the micro-nano iron plate of high activity come efficient catalytic sodium peroxydisulfate, so as to effectively degradation soil middle and high concentration PAHs（201.1 mg/kg）.The reagent combination of this micro-nano iron plate activation persulfate, can not only be under the conditions of the lab scale of laboratory to the efficient degradation of PAHs, and can be in pilot scale scale（360 cubes of soil）Rapidly and efficiently in-situ immobilization high concentration PAHs contaminated soils, and after environmental-friendly reparation soil enzyme activities index without significant changes.The reparation medicament is suitable for the reparation of high concentration PAHs contaminated soils in place in situ, efficient, easy to operate, environmental-friendly, and wide prospect is provided to repair high concentration PAHs contaminated soils.
Description
Technical field
The invention belongs to soil pollution recovery technique fields, and in particular to a kind of in-situ immobilization high concentration is polycyclic aromatic hydrocarbons contaminated
The medicament of soil and its application.
Background technology
With industry, the aggravation of municipal pollution and agricultural chemicals type, the increase of quantity, soil pollution, which has become, to be received
The global problem of environmental pollution of concern.Show that the U.S. possesses contaminated site 29.4 ten thousand at present according to U.S. EPA statistical data,
Rehabilitation expense between 2004~2033 years is expected will be up to two $ 100 billions.And in China, with " moving back two into three " and " move back city into
The steady implementation of garden " policy, the contaminating enterprises such as chemical industry, printing and dyeing in nearly all main city zone are all moved into development zone or industry
Garden, so as to cause a large amount of heavily contaminated places are emerged in large numbers in city, there are about 30~50 for current China's contaminated site according to incompletely statistics
Ten thousand.Government or soil owner are when to these land developments and recycling, it is necessary to which contaminated site soil is assessed and repaiied
It is multiple, it usually requires that and reaches reparation desired value in a short time.Therefore, efficient, low cost and environmentally friendly soil remediation is developed
Reagent combination is the Major Strategic Demand of current national development.
Polycyclic aromatic hydrocarbon (Polycyclic aromatic hydrocarbons, PAHs) refer to 2 or 2 or more phenyl ring with
Linear, horn shape or tufted permutation and combination into fused ring compound, since PAHs has high toxicity, environmental persistence, bioaccumulation
Property and " three cause " property, soil contamination problem is especially prominent, in April, 2014 Chinese Ministry of Environmental Protection's joint Ministry of Land and Resources soil pollution tune
Look into report now, the point position exceeding standard rate of PAHs contaminated soils is 1.4%, and serious threat ecological environment, food security and human body are good for
Health.Therefore, there is an urgent need for develop the recovery technique of place PAHs contaminated soils.Include currently for polycyclic aromatic hydrocarbons contaminated treatment technology
Microorganism remediation, phytoremediation and Soil leaching etc., but Yi Shang technology has the respective scope of application.Such as microorganism remediation technology
It is current most widely used PAHs recovery techniques, as Chinese patent 201610438092.0 is reported with chitin, zeolite powder
Etc. the microbial bacterial agents of compoundings effectively can degrade or adsorb PAHs in soil；Chinese patent 201010547623.2 utilizes purple
Russian fenugreek herb, arbuscular mycorrhiza and bacillus, mating surface activating agent rhamnolipid realize the degradation of PAHs in soil.It is although micro-
Biology, plant can remove the PAHs in soil, but such technology is suitable only for the reparation of farmland low concentration PAHs contaminated soils,
And repairing efficiency is longer, is not suitable for repairing the reparation of high concentration PAHs contaminated soil of site in the short time.In addition, Soil leaching is only
It can realize that PAHs is shifted, eluent needs after-treatment, and cost is higher.There is an urgent need for develop for the efficient of PAHs contaminated site soil
Recovery technique.
Chemical oxidation techniques provide new opportunity for the reparation in high concentration organic contamination place, and main mechanism is to pass through
Oxidant direct oxidation induces the chain reaction of free radical to realize the degradation to pollutant, and common oxidant has Fenton
Reagent, ozone and persulfate etc..But different type oxidant and free radical are to the reactivity difference of different type pollutant
It is larger, it is contemplated that larger in the otherness of actual place contaminated soil, it is necessary to which that exploitation is for different type pollutant and soil
The reagent combination of matter.At present, the basic research of chemical oxidation techniques degradation PAHs, but research mostly have been utilized both at home and abroad
The research of water solution system or laboratory scale is all concentrated on, is as a result difficult to be generalized in practical application.More importantly utilize
High-activity nano material couple persulfate realize in soil and pilot scale scale on PAHs reparation research not yet.
Invention content
The technical issues of solution：The present invention is directed to the great demand of high concentration polycyclic aromatic hydrocarbon contaminated soil of site reparation, opens
The engineering mimoir of micro-nano iron plate activation sodium peroxydisulfate in-situ immobilization PAHs contaminated site soil on pilot scale scale has been opened up, provides one
The medicament of kind in-situ immobilization high concentration polycyclic aromatic hydrocarbon pollution and its application, for efficiently repairing high concentration PAHs Pollution Fields
Ground.
Technical solution：A kind of medicament of in-situ immobilization high concentration polycyclic aromatic hydrocarbon pollution, active ingredient are micro-nano iron
Piece and sodium peroxydisulfate.
Preferably, the medicament of above-mentioned in-situ immobilization high concentration polycyclic aromatic hydrocarbon pollution is by micro-nano iron plate and sodium peroxydisulfate
Composition.
Preferably, the molar ratio of above-mentioned micro-nano iron plate and sodium peroxydisulfate is 1:20~2:1.
Preferably, the thickness of above-mentioned micro-nano iron plate be 35~55nm, a diameter of 3~5 μm, specific surface area 16m2/g。
Above-mentioned medicament repairs the application in high concentration polycyclic aromatic hydrocarbon pollutant in situ.
Applying step is：After places polluted by polynuclear aromatic hydrocarbons excavates reaction in-situ pond, pollutant soil is backfilled, is first added in
It after sodium peroxydisulfate stirs evenly, adds micro-nano iron plate suspension and stirs evenly, the sodium peroxydisulfate dosage is 54kg/ cubes
Soil, the dosage of micro-nano iron plate is 6.3kg/ cubes of soil, is reacted under natural conditions.
Preferably, in above-mentioned contaminated soil PAHs a concentration of 201.1mg/kg, reaction continue for 180 days.
Specifically：(1) laboratory lab scale medicament ratio is screened：The polycyclic aromatic hydrocarbon containing high concentration acquired to actual place is dirty
Micro-nano iron plate suspension and persulfate solution are added in the soil of dye, the dosage of the micro-nano iron plate is 0.35~7.0g/
The ratio of kg, a concentration of 7.5~60g/kg of sodium peroxydisulfate, micro-nano iron plate and persulfate is 1:20~2:1, it is placed in incubator
Middle concussion is 150rpm in rotating speed, and temperature is reacted under the conditions of being 25 DEG C；(2) medicament pilot scale is demonstrated：In practical polycyclic aromatic hydrocarbon
Contaminated site realizes the reparation of the soil in a manner that strange land in situ is stirred.Reaction in-situ pond is built by earthwork construction operation
Afterwards, pollutant soil layering is backfilled, after first addition sodium peroxydisulfate medicament stirs evenly, it is equal adds the stirring of micro-nano iron plate suspension
Even, the sodium peroxydisulfate dosage is 54kg/ cubes of soil, and the dosage of micro-nano iron plate is 6.3kg/ cubes of soil, anti-under natural conditions
It should.A concentration of 201.1mg/kg 23.2mg/kg of P in soil AHs, react 7 Hes respectively in above-mentioned pilot plant test and pilot scale demonstration
180 days.
Medicament repair polycyclic aromatic hydrocarbon key reaction principle be：Zero-valent Iron in micro-nano iron plate surface or lattice (represents
For ≡ Fe0) by corroding (equation 1), oxygen (equation 2) and persulfate oxidation (equation 3) effect generation surface ferrous iron (≡ Fe2 +), while surface ≡ Fe0Electronics can also be transmitted and give over cure acid ion (S2O8 2-) generation potentiometric titrations (SO4 ·-) (equation
4).By the surface ≡ Fe for reacting 1-4 generations2+A part passes to over cure acid ion (S by single electron2O8 2-) generation SO4 ·-
(equation 5), a part of SO4 ·-With H2O reaction generation hydroxyls, two kinds of free-radical oxidation mineralising PAHs generate carbon dioxide and water,
Realize the efficient degradation of PAHs.
Fe0→Fe2++2e (1)
2Fe0+O2+2H2O→2Fe2++4-OH (2)
Under soil environment condition, over cure acid ion and above-mentioned reaction are generated free radicals in PAHs degradation processes,
It can have an effect with the soil organism, decompose organic matter so as to so that the PAHs with organically-bound is released, so as to
Improve the validity and remediation efficiency of PAHs.
Advantageous effect：(1) the present invention is based on the micro-nano iron plate catalysis sodium peroxydisulfates of high activity to generate the sulphur of strong oxidizing property
Acid group free radical and hydroxyl, the generation rate of free radical is fast, utilization rate is high, system all has greater activity in the soil, to small
Soil middle and high concentration PAHs has higher removal effect under examination and pilot plant conditions.(2) the present invention is based on the catalysis of micro-nano iron plate
Reparation of the sodium peroxydisulfate to soil middle and high concentration PAHs on pilot scale scale, with more practical practicality and engineering value, PAH's is total
Concentration is up to 201.1mg/kg, and there are about 9 kinds to include for type：2- methyl naphthalenes (62.8mg/kg), benzo [a] anthracene (32.6mg/
Kg), benzo [b] fluoranthene (25.4mg/kg), benzo [k] fluoranthene (23.1mg/kg), benzo [a] pyrene (30.7mg/kg), indeno
[1,2,3-cd] pyrene (22.5mg/kg), dibenzo [a, h] anthracene (4.0mg/kg).(3) the micro-nano iron plate in the method for the present invention and
The dosage of sodium peroxydisulfate is relatively low, and reaction condition is mild, and high concentration PAHs contaminated sites can be efficiently repaired in room temperature, natural conditions
Soil.(4) the technology of the present invention is environmental-friendly, does not have a significant impact under the dosing of pilot plant conditions to soil enzyme activities,
And the reagent combination is finally decomposed to iron and sulfate ion.(5) the technology of the present invention is easy to operate, can realize contaminated sites soil
The in-situ immobilization of earth, under environmental perturbation, persistence is good, efficient, economically feasible, is suitable for repairing for all kinds of PAHs contaminated sites
It is multiple.
Description of the drawings
The removal effect figure that Fig. 1 is PAHs in soil under pilot plant conditions.
Specific embodiment
Below by embodiment, the invention will be further described, illustrates outstanding feature and the marked improvement of the present invention, only
It indicates that the present invention and is not limited to following instance.Method using the present invention is to the PAHs contaminated soil of site of high concentration
It is repaired.
Embodiment 1：
Under the conditions of the lab scale of laboratory, the dosage for having investigated micro-nano iron plate is catalyzed it PAHs in persulfate degradation soil
The influence of degradation efficiency.
Using practical PAHs contaminated sites soil as research object, using micro-nano iron plate catalytic activation sodium peroxydisulfate (PS)
In heterogeneous reaction, using the 250mL browns serum bottle with polytetrafluoroethylene (PTFE) plug as reactor, weigh 100g soil and
Reaction solution 100mL is added in, the initial concentration of persulfate is 30g/kg (126mM), and the initial dosage of micro-nano iron plate is distinguished
For 0.35 (6.3mM), 0.70 (12.6mM), 1.4 (25.2mM), 3.5 (63mM) and 7.0g/kg (126mM), micro-nano iron plate with
Sodium peroxydisulfate molar ratio is respectively 1:20、1:10、1:5、1:2 and 1:1, the concentration 201.1mg/kg of PAHs in contaminated soil,
Soil ratio 1:1, reaction bulb is placed in concussion bed, rotating speed 150rpm, temperature is 25 DEG C.The organic dirt in independent place is set simultaneously
The common Fenton reagent of soil remediation is contaminated as control, a concentration of 126mM of hydrogen peroxide, the molar ratio with ferrous ion
It is 5:1.
It is individually added into the micro-nano iron plate experiments of 7.0g/kg, does not need to add in sodium peroxydisulfate, other conditions are same as above.
It is individually added into the experiment of 30g/kg sodium peroxydisulfates, does not need to add in micro-nano iron plate, other conditions are same as above.
Processing time is 7 days, and handling result is shown in Table 1.
The result shows that with the increase of micro-nano iron plate dosage, the removal rate of 9 kinds of PAHs all increases in significant,
Dosage from 0.35 increase to 3.5g/kg when, total removal rate of PAHs increases to 42.2% from 15.3%, continues to increase micro-nano
The dosage of iron plate is to 7.0g/kg, and the removal rate increase of PAHs is not notable, and this illustrates under the conditions of this, micro-nano iron plate is most
Excellent dosage is 3.5g/kg.Meanwhile independent sodium peroxydisulfate or micro-nano iron plate or Fenton reagent are poor to the removal effect of PAHs.
Illustrate the high efficiency of micro-nano iron plate/sodium peroxydisulfate reagent combination.
Influence of the 1 micro-nano iron plate dosage of table to PAHs removal rates
Embodiment 2：
Using practical PAHs contaminated sites soil as research object, shadow of the sodium peroxydisulfate dosage to PAHs removal efficiency is had studied
It rings.
In heterogeneous reaction using micro-nano iron plate catalytic activation sodium peroxydisulfate (PS), using with polytetrafluoroethylene (PTFE) plug
250mL browns serum bottle as reactor, weigh the soil of 100g and add in reaction solution 100mL, micro-nano iron plate it is initial
Dosage is 3.5g/kg (63mM), and the initial concentration of sodium peroxydisulfate is 7.5 (31.5), 15 (63mM), 30 (126mM), 60g/kg
(252mM), the molar ratio of sodium peroxydisulfate and micro-nano iron plate is respectively 1:2、1:1、2:1 and 4:1, PAHs in contaminated soil
Concentration 201.1mg/kg, soil ratio 1:1, reaction bulb is placed in concussion bed, rotating speed 150rpm, temperature is 25 DEG C.
It is individually added into the micro-nano iron plate experiments of 3.5g/kg, does not need to add in sodium peroxydisulfate, other conditions are same as above.
It is individually added into the experiment of 60g/kg sodium peroxydisulfates, does not need to add in micro-nano iron plate, other conditions are same as above.
Processing time is 7 days, and handling result is shown in Table 2.
The result shows that with the increase of sodium peroxydisulfate concentration, the removal rate of PAHs is consequently increased, the concentration of sodium peroxydisulfate
When increasing to 30g/kg from 7.5, the removal rate of PAHs increases to 42.2% from 14.2%, continues to increase sodium peroxydisulfate concentration extremely
The removal rate of 60g/kg, PAHs only increase by 9%, and the optimum amount this illustrates persulfate is 30g/kg.
Influence of the 2 sodium peroxydisulfate dosage of table to PAHs removal rates
Embodiment 3：
The optimum amount point of the sodium peroxydisulfate that lab scale (embodiment 1 and embodiment 2) screens in laboratory and micro-nano iron plate
It Wei not 30 and 3.5g/kg (molar ratios 2:1) on the basis of, pilot scale demonstration project has been carried out.
Certain PAHs contaminated site is selected, a concentration of 201.1mg/kg of total PAHs, the area of pilot scale is 90 square metres, pollution
Depth for 4 meters of depths, total earth volume is 360 cubes.Specific place step is as follows：It is first on the basis of prepartion of land early period
It first passes through after earthwork construction operation builds reaction in-situ pond, pollutant soil is backfilled, it is equal first to add in the stirring of sodium peroxydisulfate medicament
It after even, add micro-nano iron plate suspension and stirs evenly, the sodium peroxydisulfate dosage is 54kg/ cubes of soil (30 × 1.8=54；1 is vertical
Necromancer=1.8 ton soil), the dosage of micro-nano iron plate is 6.3kg/ cubes of soil (3.5 × 1.8=6.3), is reacted under natural conditions.
Experiment compares the removal efficiency of PAHs in different time, as shown in table 3, it can be seen that with the reaction time
Increase, the removal effect of main PAHs and total PAHs all increases trend in significant in 9, and after reaction 30 days, total PAHs's goes
Except rate is up to 58.%, after reaction 100 days, the removal rate of PAHs is up to 87.2%, and end reaction is after 180 days, in soil thus
Polycyclic aromatic hydrocarbon is all substantially removed, and the concentration residual of PAHs has reached reparation desired value (exhibition use in the place soil
Ground evaluation criteria of soil environment quality (provisional)).
The removal rate of 3 pilot scale of table demonstration PAHs
Meanwhile the index of soil enzyme is analyzed in pilot scale repair process, pacified with evaluating this ecology for repairing formula
Quan Xing, the results are shown in Table 4, it can be seen that and the variation of urase, phosphatase and catalase is not notable in entire repair process,
It illustrates that this medicament does not have a significant impact to the ecological functions of this soil, illustrates the medicament for nanometer iron plate/sodium peroxydisulfate
Formula is milder, smaller to the disturbance of soil.
The variation of 4 pilot scale of table demonstration soil enzyme activities
Claims (7)
1. a kind of medicament of in-situ immobilization high concentration polycyclic aromatic hydrocarbon pollution, it is characterised in that active ingredient is micro-nano iron plate
And sodium peroxydisulfate.
2. the medicament of in-situ immobilization high concentration polycyclic aromatic hydrocarbon pollution according to claim 1, it is characterised in that by micro-nano
Rice iron plate and sodium peroxydisulfate composition.
3. the medicament of in-situ immobilization high concentration polycyclic aromatic hydrocarbon pollution according to claim 2, it is characterised in that micro-nano
The molar ratio of iron plate and sodium peroxydisulfate is 1:20~2:1.
4. the medicament of in-situ immobilization high concentration polycyclic aromatic hydrocarbon pollution according to claim 3, it is characterised in that described micro-
The thickness of nanometer iron plate is 35~55 nm, and a diameter of 3~5 μm, specific surface area is 16 m2/g。
5. any medicament of claim 1 ~ 4 repairs the application in high concentration polycyclic aromatic hydrocarbon pollutant in situ.
6. application according to claim 5, it is characterised in that step is：Reaction in-situ is excavated in places polluted by polynuclear aromatic hydrocarbons
Chi Hou backfills pollutant soil, after first addition sodium peroxydisulfate stirs evenly, adds micro-nano iron plate suspension and stirs evenly,
The sodium peroxydisulfate dosage is 54 kg/ cubes of soil, and the dosage of micro-nano iron plate is 6.3 kg/ cubes of soil, anti-under natural conditions
It should.
7. application according to claim 6, it is characterised in that a concentration of 201.1 mg/kg of PAHs in contaminated soil, instead
It should continue for 180 days.
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| CN108568451A (en) * | 2018-03-15 | 2018-09-25 | 中国科学院南京土壤研究所 | A method of repairing polycyclic aromatic hydrocarbon pollution |
| CN109304362A (en) * | 2018-10-12 | 2019-02-05 | 南京农业大学 | A method of polycyclic aromatic hydrocarbon composite pollution soil is repaired using potentiometric titrations high-level oxidation technology |
| CN110589951A (en) * | 2019-09-19 | 2019-12-20 | 大连理工大学 | Method for degrading polycyclic aromatic hydrocarbon by activating persulfate through zero-valent iron |
| CN111069274A (en) * | 2019-12-17 | 2020-04-28 | 中国科学院南京土壤研究所 | Nano-bioremediation method for soil in high-concentration polycyclic aromatic hydrocarbon contaminated site |
| CN111760899A (en) * | 2020-06-22 | 2020-10-13 | 南京农业大学 | Feeding improvement method for repairing toxic organic contaminated soil through oxidant compounding oxidation |
| CN111940490A (en) * | 2020-08-14 | 2020-11-17 | 莆田海关综合技术服务中心 | Remediation method for heavy metal and polycyclic aromatic hydrocarbon compound pollutants in soil |
| CN113030432A (en) * | 2020-05-18 | 2021-06-25 | 北京航空航天大学 | Testing device and repairing method for continuously repairing organic matter contaminated soil |
| CN114951260A (en) * | 2022-06-22 | 2022-08-30 | 昆明理工大学 | Method for restoring organic contaminated soil by using plants rich in polyphenol |
| CN114985442A (en) * | 2022-04-22 | 2022-09-02 | 东南大学 | Method for repairing polycyclic aromatic hydrocarbon polluted soil by oxidation of activated persulfate |
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| CN109304362B (en) * | 2018-10-12 | 2021-01-05 | 南京农业大学 | Method for repairing polycyclic aromatic hydrocarbon composite polluted soil by sulfate radical advanced oxidation technology |
| CN110589951A (en) * | 2019-09-19 | 2019-12-20 | 大连理工大学 | Method for degrading polycyclic aromatic hydrocarbon by activating persulfate through zero-valent iron |
| CN111069274A (en) * | 2019-12-17 | 2020-04-28 | 中国科学院南京土壤研究所 | Nano-bioremediation method for soil in high-concentration polycyclic aromatic hydrocarbon contaminated site |
| CN111069274B (en) * | 2019-12-17 | 2021-08-10 | 中国科学院南京土壤研究所 | Nano-bioremediation method for soil in high-concentration polycyclic aromatic hydrocarbon contaminated site |
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| CN113030432A (en) * | 2020-05-18 | 2021-06-25 | 北京航空航天大学 | Testing device and repairing method for continuously repairing organic matter contaminated soil |
| CN111760899A (en) * | 2020-06-22 | 2020-10-13 | 南京农业大学 | Feeding improvement method for repairing toxic organic contaminated soil through oxidant compounding oxidation |
| CN111940490A (en) * | 2020-08-14 | 2020-11-17 | 莆田海关综合技术服务中心 | Remediation method for heavy metal and polycyclic aromatic hydrocarbon compound pollutants in soil |
| CN114985442A (en) * | 2022-04-22 | 2022-09-02 | 东南大学 | Method for repairing polycyclic aromatic hydrocarbon polluted soil by oxidation of activated persulfate |
| CN114951260A (en) * | 2022-06-22 | 2022-08-30 | 昆明理工大学 | Method for restoring organic contaminated soil by using plants rich in polyphenol |
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Application publication date: 20180629 |