CN114907856A - Green and efficient polycyclic aromatic hydrocarbon contaminated soil remediation eluent and application method thereof - Google Patents
Green and efficient polycyclic aromatic hydrocarbon contaminated soil remediation eluent and application method thereof Download PDFInfo
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- CN114907856A CN114907856A CN202210524946.2A CN202210524946A CN114907856A CN 114907856 A CN114907856 A CN 114907856A CN 202210524946 A CN202210524946 A CN 202210524946A CN 114907856 A CN114907856 A CN 114907856A
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- C09K17/14—Soil-conditioning materials or soil-stabilising materials containing organic compounds only
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
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Abstract
The invention discloses a green and efficient polycyclic aromatic hydrocarbon contaminated soil remediation eluent and an application method thereof, and belongs to the technical field of field soil remediation. According to the invention, through screening of proper eluting agent components and scientific setting of the eluting agent component proportion, the solid-liquid ratio and the eluting time, green and efficient eluting remediation of the polycyclic aromatic hydrocarbon in the soil is effectively realized, and the problems of poor eluting effect, long-term residue of the active components of the eluting agent, toxicity and the like in the existing eluting remediation of the polycyclic aromatic hydrocarbon-polluted soil are solved.
Description
Technical Field
The invention belongs to the technical field of field soil remediation, and particularly relates to a green and efficient polycyclic aromatic hydrocarbon contaminated soil remediation eluent and an application method thereof.
Background
Polycyclic Aromatic Hydrocarbons (PAHs) are persistent organic pollutants composed of 2 or more than 2 benzene rings combined together in linear, angular or cluster form, and are byproducts of incomplete combustion or pyrolysis of organic matter. Most PAHs are light yellow or colorless crystals and have the characteristics of high boiling point, high melting point, low water solubility and the like. PAHs have strong inertia and stable chemical property and are widely present in various environmental media. Certain high molecular weight PAHs have been shown to have "triprodogenic" effects, such as carcinogenesis, teratogenicity, mutagenicity, and the like, and have received much attention. PAHs are primarily derived from the synthesis of biological metabolism, the synthesis of geochemical interactions from fossil fuels and minerals, and human activities. In recent years, the content of PAHs in the environment is greatly increased due to the activity of human beings, and the PAHs become a main source in the environment. Although the polycyclic aromatic hydrocarbon is less in the environment, the polycyclic aromatic hydrocarbon is widely distributed in the air, soil and water, enters the human body through the ways of breathing, diet and the like and is enriched, thereby being harmful to the health of the human body. About 90% of PAHs in the environment exist in soil, and the PAHs can affect the composition, structure and soil enzyme activity of soil microorganisms, further affect the structure and function of a soil ecosystem and cause serious pressure on soil microbial communities.
At present, the leaching remediation method is one of the methods with good effect for removing the polycyclic aromatic hydrocarbon pollutants in the soil, but the effect in the actual leaching process is often poor due to the strong hydrophobicity of the polycyclic aromatic hydrocarbon. The surfactant is a natural or artificial amphipathic molecule which can reduce the surface tension of a solvent by adding a small amount of the surfactant, and the state of a system interface is changed so as to generate the effects of wetting, dispersing, emulsifying, solubilizing and the like. At present, China has achieved some achievements in the aspect of remediation of organic contaminated soil by applying a surfactant, but the problems still exist in the remediation of organic contaminated soil by using an eluting agent, the eluting agent selection needs to be comprehensively considered in the face of complex conditions such as soil physicochemical properties and pollutant characteristics, and the problems of unstable performance and poor eluting effect still exist in the actual eluting process. Meanwhile, the residue and toxicity of the active ingredients of the eluting agent also bring the problem of secondary pollution to the environment. Therefore, the development of the polycyclic aromatic hydrocarbon polluted soil remediation eluent capable of effectively realizing efficient leaching remediation of the polycyclic aromatic hydrocarbon in the soil is urgently needed.
Disclosure of Invention
1. Problems to be solved
Aiming at the problems of poor leaching effect, long-term residue of active ingredients of the leaching agent, toxicity and the like of the existing leaching remediation method for the soil polluted by the polycyclic aromatic hydrocarbon, the invention provides the green and efficient leaching agent for the remediation of the soil polluted by the polycyclic aromatic hydrocarbon and the application method thereof. According to the invention, through screening appropriate eluting agent components and scientifically setting the proportion, solid-to-liquid ratio and eluting time of the eluting agent components, the green and efficient eluviation remediation of the polycyclic aromatic hydrocarbon in the soil is effectively realized.
2. Technical scheme
In order to solve the problems, the technical scheme adopted by the invention is as follows:
the invention relates to a polycyclic aromatic hydrocarbon contaminated soil remediation eluent, which comprises plant polyene phenol polyoxyethylene ether and polyethylene glycol as effective components, wherein the mass ratio of the plant polyene phenol polyoxyethylene ether to the polyethylene glycol is 9: 5-45: 1.
preferably, the eluent comprises the following components in percentage by mass: 0.18% -0.9%, polyethylene glycol: 0.02% -0.1%, water: 99.8 to 99 percent.
The method for restoring the soil polluted by the polycyclic aromatic hydrocarbon comprises the step of contacting the eluting agent with the soil polluted by the polycyclic aromatic hydrocarbon to elute and restore the soil polluted by the polycyclic aromatic hydrocarbon.
Preferably, the method for remedying the polycyclic aromatic hydrocarbon-polluted soil specifically comprises the following steps:
s10, removing impurities from the polycyclic aromatic hydrocarbon polluted soil, grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at-20 ℃ for later use;
s20, placing the polycyclic aromatic hydrocarbon polluted soil in the step S10 into a container, adding an eluting agent, and eluting and repairing the soil at 25 ℃;
s30, centrifuging, standing to obtain a soil-water separation substance, freeze-drying the repaired soil sample, extracting polycyclic aromatic hydrocarbons by adopting ultrasonic, purifying the extract by adopting a solid phase extraction column, and measuring polycyclic aromatic hydrocarbon residue by using a liquid chromatograph to obtain the polycyclic aromatic hydrocarbon removal rate.
Preferably, the solid-liquid ratio between the polycyclic aromatic hydrocarbon contaminated soil and the eluting agent is 1: 20-1: 80.
preferably, the leaching time is 4-24 hours.
Preferably, the mass concentration of the active ingredients of the eluting agent is 5 g/L-10 g/L.
More preferably, the solid-to-liquid ratio between the polycyclic aromatic hydrocarbon-contaminated soil and the eluting agent is 1: 40.
more preferably, the rinsing time is 12 hours.
Preferably, the polycyclic aromatic hydrocarbon polluted soil contains 100-1000 ppm of polycyclic aromatic hydrocarbon.
3. Advantageous effects
Compared with the prior art, the invention has the beneficial effects that:
(1) according to the invention, the fully biodegradable plant-derived nonionic surfactant, namely plant polyene phenol polyoxyethylene ether, is used as an active ingredient, and the eluent also comprises biodegradable polyethylene glycol, so that the high-efficiency removal of the polycyclic aromatic hydrocarbon polluted soil with high content of 100-1000 ppm is realized by reasonably setting the proportion relationship among the components of the eluent, and the removal rate of the polycyclic aromatic hydrocarbon is up to more than 75%;
(2) according to the invention, the problem of secondary pollution caused by applying a traditional surfactant to repair the soil polluted by the polycyclic aromatic hydrocarbon is avoided, and the eluent has the advantages of environmental friendliness, complete biodegradability, excellent emulsifying dispersibility, good detergency, low foam and the like;
(3) according to the method for repairing the soil polluted by the polycyclic aromatic hydrocarbon, the polycyclic aromatic hydrocarbon in the soil can be efficiently removed under the conditions of a certain eluent ratio, a certain solid-liquid ratio and a certain leaching time, meanwhile, the residual effective components of the leaching agent can be efficiently biodegraded under natural conditions, and the biodegradation degree of the soil on the seventh day is 100%.
Drawings
FIG. 1 is a graph illustrating the elution effect of various eluents of example 1 of the present invention on polycyclic aromatic hydrocarbons from soil;
FIG. 2 is a schematic illustration of the elution effect of polycyclic aromatic hydrocarbons from different solid-liquid ratios in soil according to example 2 of the present invention;
FIG. 3 is a graph showing the effect of the concentration of active ingredients in different eluents of example 3 of the present invention on the elution of polycyclic aromatic hydrocarbons from soil;
fig. 4 is a schematic diagram of the elution effect of different elution times on soil polycyclic aromatic hydrocarbons in example 4 of the present invention.
Detailed Description
The structure, proportion, size and the like shown in the drawings are only used for matching with the content disclosed in the specification, so that the person skilled in the art can understand and read the description, and the description is not used for limiting the limit condition of the implementation of the invention, so the method has no technical essence, and any structural modification, proportion relation change or size adjustment still falls within the scope covered by the technical content disclosed by the invention without affecting the effect and the achievable purpose of the invention. Meanwhile, the embodiments of the present invention are not independent of each other, but may be combined.
The invention is further described with reference to specific examples.
Example 1
The method for repairing polycyclic aromatic hydrocarbon contaminated soil comprises the following specific steps:
s10, removing impurities from the soil polluted by polycyclic aromatic hydrocarbons (PHE, PYR and BaP), grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at-20 ℃ for later use;
s20, placing 1g of polluted soil into a 50mL centrifuge tube, and adding an eluent, wherein the eluent comprises 0.45 mass percent of plant polyene phenol polyoxyethylene ether, 0.05 mass percent of polyethylene glycol and 99.5 mass percent of water, and the mass concentration of active ingredients of the eluent is 5 g/L; setting the solid-liquid ratio as 1: 40, 3 replicates were set up per sample; then placing the centrifugal tube on a constant temperature shaking bed, and horizontally shaking for 12h (25 ℃, 150 r/min);
s30, centrifuging the centrifuge tube at a high speed (3000r for 10min), standing to obtain a soil-water separation substance, ultrasonically extracting a repaired soil sample for 1h by adopting 10mL of an extracting agent (n-hexane: dichloromethane: 1), allowing 5mL of lower-layer extract to pass through a solid-phase extraction column (SPE, wherein the solid-phase extraction column is filled with 1g of anhydrous sodium sulfate/silica gel/Flori silica/anhydrous sodium sulfate from bottom to top), concentrating the purified solution on a rotary evaporator to 2mL again, adding 1mL of acetonitrile to concentrate to less than 1mL, fixing the volume to 1mL by using acetonitrile, and measuring the polycyclic aromatic hydrocarbon removal rate by upper liquid-phase chromatography to be more than 75%.
Example 2
The basic contents of this embodiment are the same as embodiment 1, except that: the method for repairing polycyclic aromatic hydrocarbon contaminated soil comprises the following specific steps:
s10, removing impurities from the soil polluted by polycyclic aromatic hydrocarbons (PHE, PYR and BaP), grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at-20 ℃ for later use;
s20, placing a certain amount of polluted soil into a 50mL centrifuge tube, and adding an eluent, wherein the eluent comprises 0.45 mass percent of plant polyene phenol polyoxyethylene ether, 0.05 mass percent of polyethylene glycol and 99.5 mass percent of water, and the mass concentration of active ingredients of the eluent is 5 g/L; the solid-liquid ratio gradient is set as 1: 100. 1: 80. 1: 50. 1: 40. 1: 20. 1: 10. 1: 5, setting 3 parallel samples for each sample; then placing the centrifugal tube on a constant temperature shaking bed, and horizontally shaking for 12h (25 ℃, 150 r/min);
s30, centrifuging the centrifuge tube at a high speed (3000r for 10min), standing to obtain a soil-water separator, performing ultrasonic extraction on the repaired soil sample to obtain polycyclic aromatic hydrocarbon, purifying the extract by using a solid phase extraction column, and determining polycyclic aromatic hydrocarbon residue by using a liquid chromatograph to obtain the polycyclic aromatic hydrocarbon removal rate.
As shown in FIG. 2, the removal rate of phenanthrene, pyrene and benzo [ a ] pyrene increases with the increase of the volume of the eluent, because the contact area of the pollutant and the surfactant is increased due to the increase of the volume of the eluent, thereby improving the elution removal efficiency. The solid-liquid ratio is from 1: 5 to 1: 100, the dosage of the leacheate is increased by 20 times, and the removal rates of phenanthrene, pyrene and benzo [ a ] pyrene are increased from 13.3%, 10.4% and 11.6% to 82.8%, 89.5% and 72.8%. Increasing the volume of the leacheate until the solid-liquid ratio is 1: at 40 hours, the removal rate of PAHs is more than 75 percent.
After that, the removal rate of PAHs increases gradually with the dosage of the eluting agent, and the removal rate of PAHs reaches 1: the removal rate at 100 hours was 85.2%. Therefore, the amount of the eluting agent added is suitably 1: 40.
example 3
The basic contents of this embodiment are the same as embodiment 1, except that: the method for repairing the polycyclic aromatic hydrocarbon-polluted soil comprises the following specific steps:
s10, removing impurities from the soil polluted by polycyclic aromatic hydrocarbons (PHE, PYR and BaP), grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at-20 ℃ for later use;
s20, placing 1g of polluted soil into a 50mL centrifuge tube, adding an eluent, wherein the eluent comprises the following components in percentage by mass: 0.08% -1.8%, polyethylene glycol: 0.02% -0.2%, water: 99.9 to 98 percent, and the concentrations of the effective components in the corresponding eluent are respectively 1g/L, 2g/L, 5g/L, 10g/L and 20 g/L. Setting the solid-liquid ratio as 1: 40, 3 replicates were set up per sample; then placing the centrifugal tube on a constant temperature shaking bed, and horizontally shaking for 12h (25 ℃, 150 r/min);
s30, centrifuging the centrifuge tube at a high speed (3000r for 10min), standing to obtain a soil-water separator, performing ultrasonic extraction on the repaired soil sample to obtain polycyclic aromatic hydrocarbon, purifying the extract by using a solid phase extraction column, and determining polycyclic aromatic hydrocarbon residue by using a liquid chromatograph to obtain the polycyclic aromatic hydrocarbon removal rate.
As shown in FIG. 3, when the concentration of the effective components of the eluting agent is 5g/L, the total PAHs removal rate reaches about 60%, and after the effective components of the eluting agent are continuously increased to 10g/L, the PAHs removal rate is more than 75%.
Example 4
The basic contents of this embodiment are the same as embodiment 1, except that: the method for repairing the polycyclic aromatic hydrocarbon-polluted soil comprises the following specific steps:
s10, removing impurities from the soil polluted by polycyclic aromatic hydrocarbons (PHE, PYR and BaP), grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at-20 ℃ for later use;
s20, placing 1g of polluted soil into a 50mL centrifuge tube, and adding an eluent, wherein the eluent comprises 0.45 mass percent of plant polyene phenol polyoxyethylene ether, 0.05 mass percent of polyethylene glycol and 99.5 mass percent of water, and the mass concentration of active ingredients of the eluent is 5 g/L; setting the solid-liquid ratio as 1: 40, 3 replicates per sample were set up; then placing the centrifugal tube on a constant temperature shaking bed, and setting the time gradient of horizontal oscillation to be 0.5h, 1h, 4h, 12h, 16h, 20h, 24h and 30h (at 25 ℃ and 150 r/min);
s30, centrifuging the centrifuge tube at a high speed (3000r for 10min), standing to obtain a soil-water separator, performing ultrasonic extraction on the repaired soil sample to obtain polycyclic aromatic hydrocarbon, purifying the extract by using a solid phase extraction column, and determining polycyclic aromatic hydrocarbon residue by using a liquid chromatograph to obtain the polycyclic aromatic hydrocarbon removal rate.
As shown in FIG. 4, the eluent of this example can only elute 51.4% of phenanthrene, 38.7% of pyrene and 34.5% of benzo [ a ] pyrene within 1h, and the average elution rate of PAHs is 41.5%. After 4h, the removal rate of PAHs gradually increases with the increase of the elution time. After the elution time reaches 12h, the removal rate of PAHs reaches a stable value (> 50%), and then the removal rate of PAHs increases slowly with time. Considering the time cost and the leaching efficiency comprehensively, the leaching time of the leaching agent is 4-24h, and the most suitable time is 12 h.
Comparative example 1
The basic contents of this comparative example are the same as example 1, except that: this comparative example provides a study of the elution effect of the following 10 eluents on soil PAHs: the eluent of example 1, Sodium Dodecyl Sulfate (SDS), Sodium Dodecyl Benzene Sulfonate (SDBS), 2-hydroxypropyl- β -cyclodextrin (HPCD), poly 23 dodecyl ether (Brij-35), Saponin (Saponin); sophorolipid (Sop) and lactone-type sophorolipid (Sop-1).
As shown in FIG. 1, the elution effect of the 10 surfactants on soil PAHs is greatly different. Wherein, the removal rate of the total PAHs of the eluent in the embodiment 1 is more than 75 percent, the removal rate of Brij-35 to the total PAHs of the soil is about 50 percent, and the removal rate of HPCD, Sop and the like to the total PAHs is less than 10 percent, and the effect is poor. The removal rate of SDS, SDBS and Sop-1 surfactant on total PAHs in soil is less than 1%, which shows that the surfactant has no elution effect on PAHs basically.
Therefore, the above results show that the eluent of example 1 has higher leaching remediation efficiency on PAHs than other commonly used commercial eluents under the same use conditions.
The invention has been described in detail hereinabove with reference to specific exemplary embodiments thereof. It will, however, be understood that various modifications and changes may be made without departing from the scope of the invention as defined in the appended claims. The detailed description and drawings are to be regarded as illustrative rather than restrictive, and any such modifications and variations are intended to be included within the scope of the present invention as described herein. Furthermore, the background is intended to be illustrative of the state of the art as developed and the meaning of the present technology and is not intended to limit the scope of the invention or the application and field of application of the invention.
More specifically, although exemplary embodiments of the invention have been described herein, the invention is not limited to these embodiments, but includes any and all embodiments modified, omitted, combined, e.g., between various embodiments, adapted and/or substituted, as would be recognized by those skilled in the art from the foregoing detailed description. The limitations in the claims are to be interpreted broadly based the language employed in the claims and not limited to examples described in the foregoing detailed description or during the prosecution of the application, which examples are to be construed as non-exclusive. Any steps recited in any method or process claims may be executed in any order and are not limited to the order presented in the claims. The scope of the invention should, therefore, be determined only by the appended claims and their legal equivalents, rather than by the descriptions and examples given above.
Claims (10)
1. The polycyclic aromatic hydrocarbon contaminated soil remediation eluent is characterized in that: the plant polyene phenol polyoxyethylene ether-polyethylene glycol compound comprises plant polyene phenol polyoxyethylene ether and polyethylene glycol as effective components, wherein the mass ratio of the plant polyene phenol polyoxyethylene ether to the polyethylene glycol is 9: 5-45: 1.
2. the polycyclic aromatic hydrocarbon-contaminated soil remediation eluent as claimed in claim 1, wherein: the eluent comprises the following components in percentage by mass: 0.18% -0.9%, polyethylene glycol: 0.02% -0.1%, water: 99.8 to 99 percent.
3. A polycyclic aromatic hydrocarbon contaminated soil remediation method is characterized in that: comprising contacting the eluent according to claim 1 or 2 with polycyclic aromatic hydrocarbon-contaminated soil to elute and repair the polycyclic aromatic hydrocarbon-contaminated soil.
4. The polycyclic aromatic hydrocarbon contaminated soil remediation method according to claim 3, wherein the method specifically comprises the following steps:
s10, removing impurities from the polycyclic aromatic hydrocarbon polluted soil, grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at-20 ℃ for later use;
s20, placing the polycyclic aromatic hydrocarbon polluted soil in the step S10 into a container, adding an eluting agent, and eluting and repairing the soil at 25 ℃;
s30, centrifuging, standing to obtain a soil-water separation substance, freeze-drying the repaired soil sample, extracting polycyclic aromatic hydrocarbons by adopting ultrasonic, purifying the extract by adopting a solid phase extraction column, and measuring polycyclic aromatic hydrocarbon residue by using a liquid chromatograph to obtain the polycyclic aromatic hydrocarbon removal rate.
5. The polycyclic aromatic hydrocarbon-contaminated soil remediation method according to claim 3, wherein: the solid-liquid ratio between the polycyclic aromatic hydrocarbon polluted soil and the eluting agent is 1: 20-1: 80.
6. the polycyclic aromatic hydrocarbon-contaminated soil remediation method according to claim 3, wherein: the leaching time is 4-24 hours.
7. The polycyclic aromatic hydrocarbon-contaminated soil remediation method according to claim 3, wherein: the mass concentration of the active ingredients of the eluting agent is 5 g/L-10 g/L.
8. The polycyclic aromatic hydrocarbon contaminated soil remediation method according to claim 5, characterized in that: the solid-liquid ratio between the polycyclic aromatic hydrocarbon polluted soil and the eluting agent is 1: 40.
9. the polycyclic aromatic hydrocarbon-contaminated soil remediation method according to claim 5, wherein: the rinsing time was 12 hours.
10. The polycyclic aromatic hydrocarbon-contaminated soil remediation method according to any one of claims 3-9, wherein: the polycyclic aromatic hydrocarbon polluted soil contains 100-1000 ppm of polycyclic aromatic hydrocarbon.
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