CN112222180A - Heavy metal lead contaminated soil remediation method based on choline chloride eutectic solvent - Google Patents
Heavy metal lead contaminated soil remediation method based on choline chloride eutectic solvent Download PDFInfo
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- CN112222180A CN112222180A CN202011053049.5A CN202011053049A CN112222180A CN 112222180 A CN112222180 A CN 112222180A CN 202011053049 A CN202011053049 A CN 202011053049A CN 112222180 A CN112222180 A CN 112222180A
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- 239000002689 soil Substances 0.000 title claims abstract description 75
- 238000000034 method Methods 0.000 title claims abstract description 27
- 229910001385 heavy metal Inorganic materials 0.000 title claims abstract description 25
- 239000001763 2-hydroxyethyl(trimethyl)azanium Substances 0.000 title claims abstract description 18
- 235000019743 Choline chloride Nutrition 0.000 title claims abstract description 18
- 229960003178 choline chloride Drugs 0.000 title claims abstract description 18
- SGMZJAMFUVOLNK-UHFFFAOYSA-M choline chloride Chemical compound [Cl-].C[N+](C)(C)CCO SGMZJAMFUVOLNK-UHFFFAOYSA-M 0.000 title claims abstract description 18
- 238000005067 remediation Methods 0.000 title claims abstract description 18
- 230000005496 eutectics Effects 0.000 title claims abstract description 16
- 239000002904 solvent Substances 0.000 title claims abstract description 16
- 238000003756 stirring Methods 0.000 claims abstract description 31
- 238000002386 leaching Methods 0.000 claims abstract description 24
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 13
- 238000010438 heat treatment Methods 0.000 claims abstract description 8
- 239000002245 particle Substances 0.000 claims abstract description 5
- 238000002156 mixing Methods 0.000 claims abstract description 3
- 238000007873 sieving Methods 0.000 claims abstract description 3
- OFOBLEOULBTSOW-UHFFFAOYSA-N Malonic acid Chemical compound OC(=O)CC(O)=O OFOBLEOULBTSOW-UHFFFAOYSA-N 0.000 claims description 14
- 239000001257 hydrogen Substances 0.000 claims description 12
- 229910052739 hydrogen Inorganic materials 0.000 claims description 12
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 claims description 9
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 8
- 239000002253 acid Substances 0.000 claims description 8
- 229910017604 nitric acid Inorganic materials 0.000 claims description 8
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 6
- DNIAPMSPPWPWGF-UHFFFAOYSA-N Propylene glycol Chemical compound CC(O)CO DNIAPMSPPWPWGF-UHFFFAOYSA-N 0.000 claims description 6
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 6
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 4
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 4
- 239000007788 liquid Substances 0.000 claims description 4
- 238000013019 agitation Methods 0.000 claims description 2
- 239000004202 carbamide Substances 0.000 claims description 2
- 238000000926 separation method Methods 0.000 claims description 2
- 239000007790 solid phase Substances 0.000 claims description 2
- 150000001875 compounds Chemical class 0.000 abstract description 2
- 238000000227 grinding Methods 0.000 abstract 1
- 239000000243 solution Substances 0.000 description 17
- 239000011259 mixed solution Substances 0.000 description 12
- 229910052751 metal Inorganic materials 0.000 description 9
- 239000000126 substance Substances 0.000 description 9
- 238000004458 analytical method Methods 0.000 description 7
- 238000001816 cooling Methods 0.000 description 7
- 238000002354 inductively-coupled plasma atomic emission spectroscopy Methods 0.000 description 7
- 239000002184 metal Substances 0.000 description 7
- 239000006228 supernatant Substances 0.000 description 7
- 238000005516 engineering process Methods 0.000 description 5
- 230000008569 process Effects 0.000 description 4
- 230000008439 repair process Effects 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000035558 fertility Effects 0.000 description 2
- WABPQHHGFIMREM-UHFFFAOYSA-N lead(0) Chemical compound [Pb] WABPQHHGFIMREM-UHFFFAOYSA-N 0.000 description 2
- 230000009471 action Effects 0.000 description 1
- 230000031018 biological processes and functions Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000011065 in-situ storage Methods 0.000 description 1
- 230000000813 microbial effect Effects 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 230000033116 oxidation-reduction process Effects 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
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Classifications
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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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- Life Sciences & Earth Sciences (AREA)
- Soil Sciences (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Processing Of Solid Wastes (AREA)
Abstract
The invention belongs to the technical field of heavy metal contaminated soil treatment, and particularly relates to a heavy metal lead contaminated soil remediation method based on a choline chloride eutectic solvent. The method comprises the steps of grinding and sieving the naturally air-dried heavy metal lead-polluted soil, mixing the sieved polluted soil particles, choline chloride eutectic solvent and dilute according to a proportion, carrying out stirring and heating leaching reaction, and eluting the lead-containing compound which is insoluble in water in the soil through stirring and heating leaching to realize effective leaching remediation of the lead-polluted soil. The method has the characteristics of simplicity, high efficiency and no secondary pollution, and has good prospect for repairing the lead-polluted soil.
Description
Technical Field
The invention belongs to the technical field of heavy metal contaminated soil treatment, and particularly relates to a heavy metal lead contaminated soil remediation method based on a choline chloride eutectic solvent.
Background
With the rapid development of industrialization and the remarkable improvement of the living standard of people, the remediation of the heavy metal contaminated soil becomes a hot spot and a difficult problem of scientific research of domestic and foreign environments.
The repair technology commonly used for heavy metal contaminated soil mainly comprises the following steps: engineering measures, physicochemical repair, chemical repair, and bioremediation techniques. The engineering measures are relatively classic soil heavy metal restoration means, and the method is simple and stable, but the method has the advantages of large engineering quantity, high investment cost, influence on the original ecological structure and soil fertility of the soil, no real removal of heavy metal substances in the soil, and treatment or stacking of the replaced polluted soil. The physical and chemical remediation technology mainly comprises three main categories of soil leaching, electric remediation and electric remediation, although the operation is simple and the implementation is convenient, the energy requirement is high, the oxidation-reduction potential of the original soil can be damaged, and the original soil ecosystem is damaged to a certain extent. The chemical remediation technology is carried out in situ on the soil, has short remediation period and is simple and easy to implement. However, chemical remediation is not a permanent removal of heavy metal harmful substances in soil, only changes the existing form of the heavy metal harmful substances in soil temporarily, and metal elements still exist in the soil environment in large quantity, and may be released again to cause harm to the environment. Moreover, the original structure of the soil can be damaged to a great extent by adding a large amount of chemical modifying agents, the soil fertility is reduced, and beneficial metal elements in the soil are reduced. Therefore, chemical remediation is often not a priority in order to take into account soil reuse and cost savings. Bioremediation is the use of biological action to restore a damaged environment, including phytoremediation and microbial remediation, at a lower cost, and does not destroy the original structure relative to other methods. But the bioremediation period is relatively long, and new biological species can be brought to the original soil ecological environment, and certain harm can be brought to an ecological system.
Disclosure of Invention
Aiming at the defects of the existing technology for repairing the lead-polluted soil, the invention aims to provide a method for repairing the lead-polluted soil based on a choline chloride eutectic solvent. The invention prepares the leaching solution by using the synthesized choline chloride eutectic solvent and the dilute nitric acid, and the metallic lead in the lead-polluted soil is successfully desorbed under the action of the leaching solution, thereby being a clean and efficient soil remediation treatment technology. The choline chloride eutectic solvent (DES for short) synthesized by the method is used for repairing heavy metal contaminated soil, is low in cost, non-toxic and biodegradable, can achieve a good repairing effect, does not have obvious influence on the original components of the soil, is efficient and green, and does not have secondary pollution.
The technical scheme adopted by the invention is as follows.
A heavy metal lead polluted soil remediation method based on choline chloride eutectic solvent comprises the following steps:
step one, taking choline chloride as a hydrogen bond acceptor (HBA for short), taking any one of malonic acid, urea, ethylene glycol, propylene glycol or glycerol as a hydrogen bond donor (HBD for short), mixing the hydrogen bond donor and the hydrogen bond acceptor in proportion, and heating in a water bath to synthesize a eutectic solvent;
step two, adding the heavy metal lead-polluted soil particles obtained through coarse crushing and sieving into a leaching solution composed of a eutectic solvent and dilute strong acid, and leaching for 0.5-6 hours at the temperature of normal temperature-40 ℃ under stirring;
and step three, after the agitation leaching is finished, carrying out solid-liquid separation, wherein a solid-phase product is the repaired soil.
In the first step, the molar ratio of the hydrogen bond acceptor to the hydrogen bond donor is 2: 1.
In the first step, the water bath heating temperature is 75-85 ℃, and the water bath heating time is 6-8 hours.
In the second step, the dilute strong acid is dilute nitric acid, dilute hydrochloric acid or dilute sulfuric acid; the mass percentage concentration of the dilute strong acid is 0.4-0.6%. The volume ratio of the eutectic solvent to the dilute strong acid is 3: 2-2: 3, and the solid-liquid mass volume ratio of the heavy metal lead polluted soil particles to the leachate is 1: 4-1: 6 g/mL.
In the second step, the stirring speed during stirring leaching is 150-300 rpm, and the stirring leaching time is 0.5-1 hour.
Compared with the prior art, the invention has the beneficial effects that:
the method can be used for efficiently treating and repairing moderate and severe lead-polluted soil. In the method, the lead polluted soil and leachate are heated and magnetically stirred, and the metallic lead existing as a compound in the soil is dissolved in H+And H3O+And the solution is replaced into an ionic state and then eluted from the soil. The raw materials for synthesizing the leaching solution required in the process have low cost and small using amount, and can be reused after being properly treated, so that the cost is reduced. In addition, the treatment method is simple and quick, has no secondary pollution in the whole process, and is a lead-polluted soil remediation method which is efficient, energy-saving, green and has an application prospect.
Drawings
FIG. 1 is a process flow diagram of the present invention.
Detailed Description
The present invention will be described in further detail with reference to the accompanying drawings and examples.
FIG. 1 is a process flow diagram of the present invention.
Example 1
The choline chloride and the malonic acid are weighed according to the molar ratio of 2: 1 and then placed in a beaker, and heated in a water bath at 80 ℃ for 7 hours to synthesize a colorless transparent solution, namely DES. DES and 0.5wt% nitric acid solution are prepared into a mixed solution according to the volume ratio of 3: 2. 10g of lead-contaminated soil (lead content about 15000 mg/kg), 50 ml of the mixed solution and a stirrer were charged into a 250 ml conical flask with a stopper. Setting the stirring speed of a magnetic stirrer to be 200 rpm, and continuously stirring for 0.5-6 hours at the temperature of 40 ℃. After the reaction is finished, the conical flask is placed at normal temperature for cooling and standing for 20 min, and the leaching concentration of the metal lead in the supernatant is analyzed by using ICP-OES.
After analysis, the lead concentration in the original soil leachate is 12533.28 mg/L after continuous stirring for 0.5 h, and 83.56 percent of lead in the soil can be removed.
Example 2
The choline chloride and the malonic acid are weighed according to the molar ratio of 2: 1 and then placed in a beaker, and heated in a water bath at 80 ℃ for 7 hours to synthesize a colorless transparent solution, namely DES. DES and 0.5wt% nitric acid solution are prepared into a mixed solution according to the volume ratio of 3: 2. 10g of lead contaminated soil (lead content about 7000 mg/kg), 50 ml of the mixed solution and a stirrer were charged into a 250 ml Erlenmeyer flask with a stopper. Setting the stirring speed of a magnetic stirrer to be 200 rpm, and continuously stirring for 0.5-6 hours at the temperature of 40 ℃. After the reaction is finished, the conical flask is placed at normal temperature for cooling and standing for 20 min, and the leaching concentration of the metal lead in the supernatant is analyzed by using ICP-OES.
After analysis, the lead concentration in the original soil leachate is 13,014.50 mg/L after continuous stirring for 0.5 h, and 85.76% of lead in the soil can be removed.
Example 3
The choline chloride and the malonic acid are weighed according to the molar ratio of 2: 1 and then placed in a beaker, and heated in a water bath at 80 ℃ for 7 hours to synthesize a colorless transparent solution, namely DES. DES and 0.5wt% nitric acid solution are prepared into a mixed solution according to the volume ratio of 3: 2. 10g of lead-contaminated soil (lead content about 15000 mg/kg), 50 ml of the mixed solution and a stirrer were charged into a 250 ml conical flask with a stopper. Setting the stirring speed of a magnetic stirrer to be 200 rpm, and continuously stirring for 0.5-6 hours at the normal temperature (25 ℃). After the reaction is finished, the conical flask is placed at normal temperature for cooling and standing for 20 min, and the leaching concentration of the metal lead in the supernatant is analyzed by using ICP-OES.
After analysis and continuous stirring for 0.5 h, the concentration of lead in the original soil leachate is 10,428.47 mg/L, and 69.52 percent of lead in the soil can be removed.
Example 4
The choline chloride and the malonic acid are weighed according to the molar ratio of 2: 1 and then placed in a beaker, and heated in a water bath at 80 ℃ for 7 hours to synthesize a colorless transparent solution, namely DES. DES and 0.5wt% hydrochloric acid solution are prepared into a mixed solution according to the volume ratio of 3: 2. 10g of lead-contaminated soil (lead content about 15000 mg/kg), 50 ml of the mixed solution and a stirrer were charged into a 250 ml conical flask with a stopper. Setting the stirring speed of a magnetic stirrer to be 200 rpm, and continuously stirring for 0.5-6 hours at the temperature of 40 ℃. After the reaction is finished, the conical flask is placed at normal temperature for cooling and standing for 20 min, and the leaching concentration of the metal lead in the supernatant is analyzed by using ICP-OES.
After analysis, the lead concentration in the original soil leachate is 12,016.95 mg/L after continuous stirring for 0.5 h, and 80.11% of lead in the soil can be removed.
Example 5
The choline chloride and the malonic acid are weighed according to the molar ratio of 2: 1 and then placed in a beaker, and heated in a water bath at 80 ℃ for 7 hours to synthesize a colorless transparent solution, namely DES. DES and 0.5wt% sulfuric acid solution are prepared into a mixed solution according to the volume ratio of 3: 2. 10g of lead-contaminated soil (lead content about 15000 mg/kg), 50 ml of the mixed solution and a stirrer were charged into a 250 ml conical flask with a stopper. Setting the stirring speed of a magnetic stirrer to be 200 rpm, and continuously stirring for 0.5-6 hours at the temperature of 40 ℃. After the reaction is finished, the conical flask is placed at normal temperature for cooling and standing for 20 min, and the leaching concentration of the metal lead in the supernatant is analyzed by using ICP-OES.
After analysis, the concentration of lead in the original soil leachate is 11,986.67 mg/L after continuous stirring for 0.5 h, and 79.91% of lead in the soil can be removed.
Example 6
The choline chloride and the glycerol are weighed according to the molar ratio of 2: 1 and then placed in a beaker, and the beaker is heated in a water bath at the temperature of 80 ℃ for 7 hours to synthesize a colorless transparent solution, namely DES. DES and 0.5wt% nitric acid solution are prepared into a mixed solution according to the volume ratio of 3: 2. 10g of lead-contaminated soil (lead content about 15000 mg/kg), 50 ml of the mixed solution and a stirrer were charged into a 250 ml conical flask with a stopper. Setting the stirring speed of a magnetic stirrer to be 200 rpm, and continuously stirring for 0.5-6 hours at the temperature of 40 ℃. After the reaction is finished, the conical flask is placed at normal temperature for cooling and standing for 20 min, and the leaching concentration of the metal lead in the supernatant is analyzed by using ICP-OES.
After analysis, the concentration of lead in the original soil leachate is 11098.32 mg/L after continuous stirring for 1 h, and 73.99% of lead in the soil can be removed.
Comparative example 1
10g of lead-contaminated soil (lead content about 15000 mg/kg), 50 ml of 0.5wt% nitric acid and a stirrer were charged into a 250 ml conical flask with a stopper. Setting the stirring speed of a magnetic stirrer to be 200 rpm, and continuously stirring for 0.5-6 hours at the temperature of 40 ℃. After the reaction is finished, the conical flask is placed at normal temperature for cooling and standing for 20 min, and the leaching concentration of the metal lead in the supernatant is analyzed by using ICP-OES.
After analysis, the lead concentration in the original soil leachate is 6308.45 mg/L after continuous stirring for 0.5 h, and 42.06% of lead in the soil can be removed.
Claims (6)
1. A heavy metal lead polluted soil remediation method based on choline chloride eutectic solvent is characterized by comprising the following steps:
step one, taking choline chloride as a hydrogen bond acceptor, taking any one of malonic acid, urea, ethylene glycol, propylene glycol or glycerol as a hydrogen bond donor, mixing the hydrogen bond acceptor and the hydrogen bond donor in proportion, and heating in a water bath to synthesize a eutectic solvent;
step two, adding the heavy metal lead-polluted soil particles obtained through coarse crushing and sieving into a leaching solution composed of a eutectic solvent and dilute strong acid, and leaching for 0.5-6 hours at the temperature of normal temperature-40 ℃ under stirring;
and step three, after the agitation leaching is finished, carrying out solid-liquid separation, wherein a solid-phase product is the repaired soil.
2. The method for remediating heavy metal lead-contaminated soil as recited in claim 1, wherein in the first step, the molar ratio of the hydrogen bond acceptor to the hydrogen bond donor is 2: 1.
3. The method for remediating heavy metal lead-contaminated soil as recited in claim 1, wherein in the first step, the water bath heating temperature is 75-85 ℃, and the water bath heating time is 6-8 hours.
4. The method for remediating heavy metal lead-contaminated soil as recited in claim 1, wherein in the second step, the dilute strong acid is dilute nitric acid, dilute hydrochloric acid, or dilute sulfuric acid; the mass percentage concentration of the dilute strong acid is 0.4-0.6%.
5. The method for remediating heavy metal lead-contaminated soil as recited in claim 1, wherein in the second step, the volume ratio of the eutectic solvent to the dilute strong acid is 3: 2 to 2: 3, and the solid-liquid mass volume ratio of the heavy metal lead-contaminated soil particles to the leachate is 1:4 to 1:6 g/mL.
6. The method for remediating heavy metal lead-contaminated soil as recited in claim 1, wherein in the second step, the stirring speed during the stirring leaching is 150-300 rpm, and the stirring leaching time is 0.5-1 hour.
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Cited By (2)
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CN113798318A (en) * | 2021-09-18 | 2021-12-17 | 云南省生态环境科学研究院 | Electrochemical remediation method of lead-zinc combined contaminated soil based on eutectic solvent |
CN113926842A (en) * | 2021-10-28 | 2022-01-14 | 东北大学 | Preparation and leaching method of high-concentration heavy metal composite contaminated soil leaching material |
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