CN114907856B - Green and efficient polycyclic aromatic hydrocarbon polluted soil restoration eluent and application method - Google Patents
Green and efficient polycyclic aromatic hydrocarbon polluted soil restoration eluent and application method Download PDFInfo
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- CN114907856B CN114907856B CN202210524946.2A CN202210524946A CN114907856B CN 114907856 B CN114907856 B CN 114907856B CN 202210524946 A CN202210524946 A CN 202210524946A CN 114907856 B CN114907856 B CN 114907856B
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Abstract
The invention discloses a green and efficient polycyclic aromatic hydrocarbon polluted soil restoration eluent and an application method thereof, and belongs to the technical field of site soil restoration. According to the invention, through screening proper leaching agent components and scientifically setting leaching agent component distribution ratio, solid-liquid ratio and leaching time, green and efficient leaching restoration of the polycyclic aromatic hydrocarbon in the soil is effectively realized, and the problems of poor leaching effect, long-term residue of active ingredients of the leaching agent, toxicity and the like in the existing leaching restoration of polycyclic aromatic hydrocarbon polluted soil are solved.
Description
Technical Field
The invention belongs to the technical field of site soil remediation, and particularly relates to a green and efficient polycyclic aromatic hydrocarbon polluted soil remediation eluent and an application method thereof.
Background
Polycyclic Aromatic Hydrocarbons (PAHs) are persistent organic pollutants composed of 2 or more benzene rings combined together in a linear, angular or clustered form, and are byproducts of incomplete combustion or pyrolysis of organic matters. Most PAHs are pale yellow or colorless crystals, and have the characteristics of high boiling point, high melting point, low water solubility and the like. PAHs are relatively inert and stable in chemical property, and widely exist in various environmental media. Certain high molecular weight PAHs have been shown to have "tri-induced" effects of carcinogenesis, teratogenicity, mutagenesis, etc., and are of great interest. PAHs are mainly derived from bio-metabolic synthesis, geochemical synthesis of fossil fuels and mineral formation, and human activities. In recent years, the content of PAHs emitted in the environment due to human activities is greatly increased, and the PAHs become a main source of the PAHs in the environment. Although the content of polycyclic aromatic hydrocarbon in the environment is small, the polycyclic aromatic hydrocarbon is widely distributed in air, soil and water, and enters the human body through respiration, diet and other ways to enrich, thereby endangering the health of the human body. About 90% of the PAHs in the environment exist in the soil, and the PAHs can influence the composition, structure and soil enzyme activity of soil microorganisms, further influence the structure and function of the soil ecosystem, and cause serious stress on soil microbial communities.
At present, the leaching repair method is one of the methods with better 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 amphiphilic molecule which can reduce the surface tension of a solvent by adding a small amount and change the interface state of a system so as to generate the functions of wetting, dispersing, emulsifying, solubilizing and the like. At present, some achievements are achieved in the aspect of repairing organic contaminated soil by using surfactants in China, but problems still exist in repairing organic contaminated soil leaching agents, and the problems of unstable performance and poor leaching effect still exist in the actual leaching process due to the fact that leaching agent selection needs to be comprehensively considered in the face of complex conditions of physical and chemical properties of soil, pollutant characteristics and the like. Meanwhile, the residue, toxicity and the like of the active ingredients of the leaching agent also bring about the secondary pollution problem of the environment. Therefore, development of a polycyclic aromatic hydrocarbon polluted soil repair eluent capable of effectively realizing efficient leaching repair of polycyclic aromatic hydrocarbons in soil is needed at present.
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 and restoring the polycyclic aromatic hydrocarbon polluted soil, the invention provides the environment-friendly and efficient polycyclic aromatic hydrocarbon polluted soil restoring leaching agent and the application method thereof. According to the invention, through screening proper leaching agent components and scientifically setting leaching agent component distribution ratio, solid-liquid ratio and leaching time, the green and efficient leaching repair of the soil polycyclic aromatic hydrocarbon is effectively realized.
2. Technical proposal
In order to solve the problems, the technical scheme adopted by the invention is as follows:
the invention relates to a polycyclic aromatic hydrocarbon polluted soil restoration eluent, which comprises plant polyene phenol polyoxyethylene ether and polyethylene glycol as active ingredients, wherein the mass ratio of the plant polyene phenol polyoxyethylene ether to the polyethylene glycol is 9:5 to 45:1.
preferably, the leacheate comprises plant polyphenol polyoxyethylene ether in mass percent: 0.18 to 0.9 percent of polyethylene glycol: 0.02% -0.1%, water: 99.8 to 99 percent.
The invention relates to a method for restoring polycyclic aromatic hydrocarbon polluted soil, which comprises the steps of contacting the eluting agent with polycyclic aromatic hydrocarbon polluted soil, and eluting and restoring the polycyclic aromatic hydrocarbon polluted soil.
Preferably, the method for repairing the polycyclic aromatic hydrocarbon polluted soil comprises the following steps of:
s10, removing impurities from polycyclic aromatic hydrocarbon polluted soil, grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at the temperature of minus 20 ℃ for later use;
s20, placing the polycyclic aromatic hydrocarbon polluted soil in the step S10 into a container, adding a eluting agent, and eluting and repairing the soil at 25 ℃;
s30, centrifuging, standing to obtain a soil-water separator, freeze-drying the repaired soil sample, ultrasonically extracting the polycyclic aromatic hydrocarbon, purifying the extract by using a solid-phase extraction column, and measuring the polycyclic aromatic hydrocarbon residue by using a liquid chromatograph to obtain the polycyclic aromatic hydrocarbon removal rate.
Preferably, the solid-to-liquid ratio between the polycyclic aromatic hydrocarbon contaminated soil and the leaching agent is 1: 20-1: 80.
preferably, the time of rinsing is 4 to 24 hours.
Preferably, the mass concentration of the active ingredients of the leaching agent is 5 g/L-10 g/L.
More preferably, the solid to liquid ratio between the polycyclic aromatic hydrocarbon contaminated soil and the leacheate is 1:40.
more preferably, the time of rinsing is 12 hours.
Preferably, the polycyclic aromatic hydrocarbon contaminated soil contains 100-1000 ppm polycyclic aromatic hydrocarbon.
3. Advantageous effects
Compared with the prior art, the invention has the beneficial effects that:
(1) According to the polycyclic aromatic hydrocarbon contaminated soil restoration eluent disclosed by the invention, a completely biodegradable plant source nonionic surfactant, namely plant polyene phenol polyoxyethylene ether is selected as an effective component, and biodegradable polyethylene glycol is also contained, so that the high-efficiency removal of the polycyclic aromatic hydrocarbon contaminated soil with the high content of 100-1000 ppm is realized by reasonably setting the proportioning relation among the components of the eluent, and the removal rate of the polycyclic aromatic hydrocarbon is as high as more than 75%;
(2) The polycyclic aromatic hydrocarbon contaminated soil restoration eluent disclosed by the invention has the advantages that the problem of secondary pollution generated when the polycyclic aromatic hydrocarbon contaminated soil is restored by using the traditional surfactant is avoided, and the eluent has the advantages of environment friendliness, complete biodegradability, excellent emulsifying dispersibility, good detergency, low foam and the like;
(3) According to the method for restoring the soil polluted by the polycyclic aromatic hydrocarbon, provided by the invention, under the conditions of a certain eluent proportion, a certain solid-liquid ratio and a certain leaching time, the polycyclic aromatic hydrocarbon in the soil can be effectively removed, meanwhile, the residual active ingredients of the leaching agent can be effectively biodegraded under the natural condition, and the biodegradation degree in the seventh day is 100%.
Drawings
FIG. 1 is a schematic diagram showing the elution effect of different leaches of example 1 of the present invention on soil polycyclic aromatic hydrocarbons;
FIG. 2 is a schematic diagram showing the effect of different solid-to-liquid ratios on the elution of soil polycyclic aromatic hydrocarbons according to example 2 of the present invention;
FIG. 3 is a graph showing the effect of the concentration of the active ingredient in the different leaches of example 3 on the elution of polycyclic aromatic hydrocarbon in soil;
fig. 4 is a schematic diagram showing the elution effect of different elution times on soil polycyclic aromatic hydrocarbon according to example 4 of the present invention.
Detailed Description
The structures, proportions, sizes, etc. shown in the drawings are shown only in connection with the present disclosure, and therefore should not be construed as limiting the invention, but rather as limiting the scope of the invention, so that any structural modifications, proportional changes, or dimensional adjustments should fall within the scope of the invention without affecting the efficacy or achievement thereof. Meanwhile, the embodiments of the present invention are not independent from each other, but may be combined.
The invention is further described below in connection with specific embodiments.
Example 1
The method for repairing the polycyclic aromatic hydrocarbon polluted soil in the embodiment comprises the following specific steps:
s10, removing impurities from the soil polluted by the polycyclic aromatic hydrocarbon (PHE, PYR, baP), grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at the temperature of minus 20 ℃ for later use;
s20, placing 1g of polluted soil into a 50mL centrifuge tube, and adding a leaching agent, wherein the leaching agent comprises 0.45% of plant polyene phenol polyoxyethylene ether, 0.05% of polyethylene glycol and 99.5% of water by mass, and the mass concentration of the active ingredients of the leaching agent is 5g/L; the solid-to-liquid ratio was set to 1:40, 3 replicates per sample were set; then placing the centrifuge tube on a constant temperature shaking table, and horizontally oscillating for 12 hours (25 ℃ and 150 r/min);
s30, centrifuging a centrifuge tube at a high speed (3000 r and 10 min), standing to obtain a soil-water separator, ultrasonically extracting a repaired soil sample for 1h by adopting 10mL of an extractant (n-hexane: dichloromethane=1:1), taking 5mL of lower layer extract, passing through a solid phase extraction column (SPE, filling the solid phase extraction column with anhydrous sodium sulfate/silica gel/florisil silica gel/anhydrous sodium sulfate from bottom to top respectively for 1 g), concentrating the purifying liquid on a rotary evaporator again to 2mL, adding 1mL of acetonitrile, concentrating to less than 1mL, fixing the volume to 1mL by acetonitrile, and measuring the polycyclic aromatic hydrocarbon removal rate by using upper liquid chromatography to be more than 75%.
Example 2
The basic content of this embodiment is the same as embodiment 1, except that: the method for repairing the polycyclic aromatic hydrocarbon polluted soil in the embodiment comprises the following specific steps:
s10, removing impurities from the soil polluted by the polycyclic aromatic hydrocarbon (PHE, PYR, baP), grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at the temperature of minus 20 ℃ for later use;
s20, placing a certain amount of polluted soil into a 50mL centrifuge tube, and adding a leaching agent, wherein the leaching agent comprises 0.45% by mass of plant polyene phenol polyoxyethylene ether, 0.05% by mass of polyethylene glycol and 99.5% by mass of water, and the mass concentration of the active ingredients of the leaching agent is 5g/L; the solid-to-liquid ratio gradient was set to 1: 100. 1:80. 1: 50. 1:40. 1: 20. 1: 10. 1:5, setting 3 parallel samples for each sample; then placing the centrifuge tube on a constant temperature shaking table, and horizontally oscillating for 12 hours (25 ℃ and 150 r/min);
s30, centrifuging the centrifuge tube at a high speed (3000 r and 10 min), standing to obtain a soil-water separator, ultrasonically extracting the polycyclic aromatic hydrocarbon from the repaired soil sample, purifying the extract by using a solid-phase extraction column, and measuring the polycyclic aromatic hydrocarbon residue by using a liquid chromatograph to obtain the polycyclic aromatic hydrocarbon removal rate.
As shown in fig. 2, as the volume of the eluent increases, the removal rates of phenanthrene, pyrene and benzo [ a ] pyrene tend to increase, because the volume of the eluent increases, the contact area of the contaminants and the surfactant increases, thereby improving the elution removal efficiency. The solid-to-liquid ratio is from 1:5 to 1:100, the usage amount of the leaching solution is increased by 20 times, and the removal rate of phenanthrene, pyrene and benzo [ a ] pyrene is increased from 13.3%, 10.4%, 11.6% to 82.8%, 89.5% and 72.8%. Increasing the volume of the eluent to a solid-liquid ratio of 1: at 40, PAHs removal was >75%.
Thereafter, the PAHs removal rate increased gradually with increasing usage of the leaching agent, and at this time, the PAHs removal rate has reached 1: the removal rate at 100 is 85.2%. Thus, suitable addition of the leaching agent is a solid to liquid ratio of 1:40.
example 3
The basic content of this embodiment is the same as embodiment 1, except that: the method for repairing the polycyclic aromatic hydrocarbon polluted soil in the embodiment comprises the following specific steps:
s10, removing impurities from the soil polluted by the polycyclic aromatic hydrocarbon (PHE, PYR, baP), grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at the temperature of minus 20 ℃ for later use;
s20, placing 1g of polluted soil into a 50mL centrifuge tube, and adding a leaching agent, wherein the leaching agent comprises plant polyene phenol polyoxyethylene ether in percentage by mass: 0.08% -1.8% of polyethylene glycol: 0.02% -0.2%, water: 99.9-98%, and the concentration of the effective components in the corresponding leacheate is 1g/L, 2g/L, 5g/L, 10g/L and 20g/L respectively. The solid-to-liquid ratio was set to 1:40, 3 replicates per sample were set; then placing the centrifuge tube on a constant temperature shaking table, and horizontally oscillating for 12 hours (25 ℃ and 150 r/min);
s30, centrifuging the centrifuge tube at a high speed (3000 r and 10 min), standing to obtain a soil-water separator, ultrasonically extracting the polycyclic aromatic hydrocarbon from the repaired soil sample, purifying the extract by using a solid-phase extraction column, and measuring the 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 eluent is 5g/L, the total PAHs removal rate reaches about 60%, and after the effective components of the eluent are continuously increased to 10g/L, the PAHs removal rate is more than 75%.
Example 4
The basic content of this embodiment is the same as embodiment 1, except that: the method for repairing the polycyclic aromatic hydrocarbon polluted soil in the embodiment comprises the following specific steps:
s10, removing impurities from the soil polluted by the polycyclic aromatic hydrocarbon (PHE, PYR, baP), grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at the temperature of minus 20 ℃ for later use;
s20, placing 1g of polluted soil into a 50mL centrifuge tube, and adding a leaching agent, wherein the leaching agent comprises 0.45% of plant polyene phenol polyoxyethylene ether, 0.05% of polyethylene glycol and 99.5% of water by mass, and the mass concentration of the active ingredients of the leaching agent is 5g/L; the solid-to-liquid ratio was set to 1:40, 3 replicates per sample were set; then placing the centrifuge tube on a constant temperature shaking table, and setting the time gradient of horizontal oscillation to be 0.5h, 1h, 4h, 12h, 16h, 20h, 24h and 30h (25 ℃ and 150 r/min);
s30, centrifuging the centrifuge tube at a high speed (3000 r and 10 min), standing to obtain a soil-water separator, ultrasonically extracting the polycyclic aromatic hydrocarbon from the repaired soil sample, purifying the extract by using a solid-phase extraction column, and measuring the polycyclic aromatic hydrocarbon residue by using a liquid chromatograph to obtain the polycyclic aromatic hydrocarbon removal rate.
As shown in FIG. 4, the eluent in the present example was able to elute only 51.4% of phenanthrene, 38.7% of pyrene and 34.5% of benzo [ a ] pyrene within 1h, and the average elution rate of PAHs was 41.5%. After 4h, the PAHs removal rate gradually increased with increasing elution time. After 12h of elution time, the PAHs removal rate reached a steady (> 50%) and thereafter increased slowly with time. Considering the time cost and the leaching efficiency comprehensively, the leaching time of the leaching agent is 4-24h, and the leaching time is most preferably 12 h.
Comparative example 1
The basic content of this comparative example is the same as in example 1, except that: this comparative example provides the following 10 eluents for examining the elution effect of soil PAHs: the eluent of example 1, sodium Dodecyl Sulfate (SDS), sodium Dodecyl Benzene Sulfonate (SDBS), 2-hydroxypropyl-beta-cyclodextrin (HPCD), poly 23 dodecyl ether (Brij-35), saponin (Saponin); sophorolipids (Sop), and endoplasmic sophorolipids (Sop-1).
As shown in fig. 1, the elution effects of these 10 surfactants on soil PAHs are greatly different. The eluent in example 1 has a total PAHs removal rate of >75%, brij-35 has a total PAHs removal rate of about 50% for soil, and HPCD, sop and the like have a total PAHs removal rate of less than 10%, which is poor in effect. The removal rate of the SDS, SDBS and Sop-1 surfactants on the total PAHs of the soil is less than 1%, which shows that the three surfactants have no elution effect on the PAHs.
Thus, the above results demonstrate that the eluent of example 1 is more effective in the leaching remediation of soil PAHs than other commercially available commonly used leaches under the same conditions of use.
The invention has been described in detail hereinabove with reference to specific exemplary embodiments thereof. It will be understood that various modifications and changes may be made without departing from the scope of the invention as defined by the appended claims. The detailed description and drawings are to be regarded in an illustrative rather than a restrictive sense, and if any such modifications and variations are desired to be included within the scope of the invention described herein. Furthermore, the background art is intended to illustrate the status and meaning of the development of the technology and is not intended to limit the invention or the application and field of application of the invention.
More specifically, although exemplary embodiments of the present invention have been described herein, the present invention is not limited to these embodiments, but includes any and all embodiments that have been modified, omitted, e.g., combined, adapted, and/or substituted between the various embodiments, as would be recognized by those skilled in the art in light of the foregoing detailed description. The limitations in the claims are to be interpreted broadly based on 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 (8)
1. A polycyclic aromatic hydrocarbon contaminated soil remediation eluent is characterized in that: the leaching agent comprises plant polyene phenol polyoxyethylene ether in percentage by mass: 0.18 to 0.9 percent of polyethylene glycol: 0.02% -0.1%, water: 99.8 to 99 percent.
2. A method for repairing soil polluted by polycyclic aromatic hydrocarbon is characterized by comprising the following steps: the method comprises the step of contacting the eluting agent according to claim 1 with polycyclic aromatic hydrocarbon polluted soil to restore the polycyclic aromatic hydrocarbon polluted soil, wherein the polycyclic aromatic hydrocarbon polluted soil contains 100-1000 ppm of polycyclic aromatic hydrocarbon.
3. The method for restoring soil polluted by polycyclic aromatic hydrocarbon according to claim 2, which is characterized by comprising the following steps:
s10, removing impurities from polycyclic aromatic hydrocarbon polluted soil, grinding, sieving with a 60-mesh sieve, and storing in a sealed brown bottle at the temperature of minus 20 ℃ for later use;
s20, placing the polycyclic aromatic hydrocarbon polluted soil in the step S10 into a container, adding a eluting agent, and eluting and repairing the soil at 25 ℃;
s30, centrifuging, standing to obtain a soil-water separator, freeze-drying the repaired soil sample, ultrasonically extracting the polycyclic aromatic hydrocarbon, purifying the extract by using a solid-phase extraction column, and measuring the polycyclic aromatic hydrocarbon residue by using a liquid chromatograph to obtain the polycyclic aromatic hydrocarbon removal rate.
4. The method for restoring soil polluted by polycyclic aromatic hydrocarbon according to claim 2, which is characterized in that: the solid-to-liquid ratio between the polycyclic aromatic hydrocarbon polluted soil and the leaching agent is 1: 20-1: 80.
5. the method for restoring soil polluted by polycyclic aromatic hydrocarbon according to claim 2, which is characterized in that: the rinsing time is 4-24 hours.
6. The method for restoring soil polluted by polycyclic aromatic hydrocarbon according to claim 2, which is characterized in that: the mass concentration of the active ingredients of the leaching agent is 5 g/L-10 g/L.
7. The method for restoring soil polluted by polycyclic aromatic hydrocarbon according to claim 4, which is characterized in that: the solid-to-liquid ratio between the polycyclic aromatic hydrocarbon polluted soil and the leaching agent is 1:40.
8. the method for restoring soil polluted by polycyclic aromatic hydrocarbon according to claim 4, which is characterized in that: the time for the rinsing was 12 hours.
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| CN102433126A (en) * | 2011-09-06 | 2012-05-02 | 浙江大学 | Natural eluting agent and method for repairing polycyclic aromatic hydrocarbon (PAH)-polluted soil |
| US9371489B2 (en) * | 2013-03-15 | 2016-06-21 | GreenStract, LLC | Plant-based compositions and uses thereof |
| CN105018101B (en) * | 2015-07-21 | 2018-06-19 | 华南理工大学 | Mixtures of eluents and its preparation and application of a kind of synchronous removal PCBs in Soil and heavy metal |
| CN105199742A (en) * | 2015-11-02 | 2015-12-30 | 张作玮 | Leaching liquid for repairing soil polluted by organic matters |
| CN107282617B (en) * | 2017-06-05 | 2020-05-19 | 浙江省环境工程有限公司 | Polycyclic aromatic hydrocarbon-heavy metal contaminated soil remediation method |
| JP7422071B2 (en) * | 2018-06-22 | 2024-01-25 | 日鉄セメント株式会社 | Heavy metal insolubilization solidification material and method for improving contaminated soil |
| CN109759427A (en) * | 2019-01-25 | 2019-05-17 | 湖南新九方科技有限公司 | The restorative procedure of PAHs contaminated soil |
| CN110918627B (en) * | 2019-11-15 | 2021-03-23 | 中国科学院南京土壤研究所 | Polycyclic aromatic hydrocarbon and chromium combined pollution soil synergistic leacheate in electroplating industry and application thereof |
| CN111495958A (en) * | 2020-04-28 | 2020-08-07 | 中国科学院过程工程研究所 | Contaminated soil remediation method |
| CN114133933A (en) * | 2020-09-04 | 2022-03-04 | 中国石油化工股份有限公司 | Eluting agent for restoring petroleum hydrocarbon contaminated soil and preparation method and application thereof |
| CN112280560B (en) * | 2020-09-28 | 2021-12-07 | 广东省环境科学研究院 | Composite eluting agent and method for eluting soil organic pollutants |
| CN113070332B (en) * | 2021-03-22 | 2022-05-20 | 华东理工大学 | Compound eluting agent for repairing polycyclic aromatic hydrocarbon contaminated soil and application thereof |
| CN113649410B (en) * | 2021-08-30 | 2022-06-10 | 湖北亮绿环保技术有限公司 | Process for repairing heavy metal pollution of soil by using nano repairing material |
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