CN112453048B - Electric in-situ remediation method for chromium-contaminated soil - Google Patents
Electric in-situ remediation method for chromium-contaminated soil Download PDFInfo
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- CN112453048B CN112453048B CN202011228942.7A CN202011228942A CN112453048B CN 112453048 B CN112453048 B CN 112453048B CN 202011228942 A CN202011228942 A CN 202011228942A CN 112453048 B CN112453048 B CN 112453048B
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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
- B09C1/085—Reclamation of contaminated soil chemically electrochemically, e.g. by electrokinetics
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
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Abstract
The invention relates to an electric in-situ remediation method for chromium-contaminated soil, which comprises the following steps: s1, adjusting the water content of chromium-polluted soil to be more than 10%; s2, introducing carbon dioxide gas into chromium-contaminated soil to protect the desorption agent sodium gluconate from biodegradation; s3, adding the sodium gluconate solution into an electric remediation cathode well of the chromium-contaminated soil; s4, applying direct current to the two electrodes arranged in the chromium-polluted soil area to electrically repair the chromium-polluted soil in situ; under the action of an electric field, the gluconate ions migrate to the anode and form a ligand with trivalent chromium-containing cations in the migration process, and the trivalent chromium is separated from insoluble precipitates or the surface of soil particles, so that the chromium in the soil polluted by the chromium is removed; and S5, adding hydrogen peroxide into the repaired soil, and removing redundant sodium gluconate. The method has the advantages of high repairing speed, high chromium pollution removal rate and no secondary pollution.
Description
Technical Field
The invention belongs to the technical field of heavy metal contaminated soil remediation, and particularly relates to an electric in-situ remediation method for chromium contaminated soil.
Background
In the process of economic development and urbanization of China, the properties of a plurality of industrial lands are changed into residential and public lands, wherein the lands are polluted by heavy metal chromium. In order to ensure the safety of public living and land use, the soil of the chromium-polluted site needs to be repaired by certain technical means to remove pollutants.
Chromium in the polluted soil generally exists in two stable valence states of trivalent and hexavalent, wherein the trivalent chromium is low in toxicity, and the hexavalent chromium is high in toxicity, has carcinogenicity, and can interfere with an enzyme system of human protein through respiratory tract and skin permeation to cause health damage. At present, two main technical routes for repairing chromium-contaminated soil are provided, including changing the valence state of chromium and removing chromium from soil. The technical route for removing chromium element from soil becomes a research hotspot because the harm of chromium pollution to soil can be fundamentally solved; the main repair technologies at present include phytoremediation, soil leaching, electric repair and the like, wherein the phytoremediation period is long, the soil leaching destroys the soil structure, and the electric in-situ repair can quickly remove chromium in the soil without damaging the soil structure, so that the technology becomes the most attractive technology for removing chromium from the polluted soil.
Electric in-situ remediationThe technology has good effect on removing anionic pollutants in soil, and hexavalent chromium mainly exists in the form of anions in the soil, including CrO 4 2- 、HCr 2 O 7 - 、Cr 2 O 7 2- And the anions are easy to dissolve in water, have good mobility and weak adsorption on most soil surfaces, so the anions containing hexavalent chromium can be directly transferred to an electrode anode for removal in the soil electrokinetic in-situ remediation process. However, heavy metal contaminants in the form of cations are often strongly adsorbed onto the surface of soil particles or form insoluble precipitates, the trivalent chromium ions being often referred to as Cr 3+ 、Cr(OH) 2 + 、Cr(OH) 2+ When the cations are adsorbed and fixed by soil particles, the carbonate and the hydroxide of the cations are difficult to dissolve in water, and the cations must be desorbed from the surface of the soil particles and separated from the difficult-to-dissolve precipitate to be brought into solution and then can be removed in an electric mode. Therefore, finding a suitable trivalent chromium desorbent becomes a difficult point for electrically repairing the chromium-polluted soil in situ.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides an electric in-situ remediation method for chromium-contaminated soil, which is characterized in that sodium gluconate is added as a desorption agent to form a ligand with trivalent chromium-containing cations, trivalent chromium is released from insoluble substances and the surfaces of soil particles to enter a solution, and the trivalent chromium is migrated under the action of an electric field, so that the chromium contamination is electrically removed from the soil in situ.
The invention is realized in such a way that an electric in-situ remediation method for chromium-contaminated soil comprises the following steps:
s1, adjusting the water content of chromium-polluted soil to be more than 10% so that pore water between electrodes is electrically connected;
s2, introducing carbon dioxide gas into the chromium-polluted soil to provide an anaerobic environment and reduce biodegradation of sodium gluconate;
s3, adding the sodium gluconate solution into an electric remediation cathode well of the chromium-contaminated soil;
s4, applying direct current to the two electrodes arranged in the chromium-polluted soil area to electrically repair the chromium-polluted soil in situ; under the action of an electric field, glucose acid radical ions migrate to the anode and form a ligand with trivalent chromium-containing cations in the migration process, and the trivalent chromium is separated from insoluble precipitates or the surface of soil particles, so that the chromium in the chromium-polluted soil is removed;
and S5, adding hydrogen peroxide into the repaired soil, and removing redundant sodium gluconate.
In the above technical solution, preferably, in the step S1, the moisture content of the chromium-contaminated soil is adjusted to be 12% or more.
In the above technical solution, preferably, in the step S2, the carbon dioxide gas introduction rate is 0.1-1.0m 3 /h。
In the above technical solution, it is further preferable that the carbon dioxide gas introduction rate is 0.5m 3 /h。
In the above technical solution, preferably, in the step S3, the concentration of the sodium gluconate solution is 0.01 to 0.1mol/L.
In the above technical solution, it is further preferable that the concentration of the sodium gluconate solution is 0.05mol/L.
In the above technical solution, preferably, in the step S4, the voltage gradient between the two electrodes is controlled to be 2.0-4.0V/cm.
In the above technical solution, it is further preferable that the voltage gradient between the two electrodes is controlled to be 3.0V/cm.
In the above technical solution, preferably, in the step S5, the concentration of hydrogen peroxide is 10%.
In order to effectively separate trivalent chromium and achieve the purpose of removing chromium pollutants under the condition of an electric field, the desorption agent sodium gluconate is added to enable gluconate ions and trivalent chromium cations to form negatively charged ligands, so that the trivalent chromium adsorbed on the surface of the chromium-polluted soil is separated from precipitates, and meanwhile, the sodium gluconate can be neutralized with hydroxide ions generated after an electrode is electrified to maintain the condition that the soil is close to neutrality, so that the adverse effect of soil acidification caused by electrolysis is avoided, and the adverse effect of the soil acidification caused by electrolysis is also avoidedH generated at cathode after electrification + And OH - The phenomenon of insufficient migration of chromium pollutants caused by transmitting most of current occurs.
The electric in-situ remediation method is suitable for a soil system with a certain water content, and requires that the pore water between the electrodes is electrically connected. By regulating and controlling the content of water in the soil, the chromium-polluted soil can be subjected to electric in-situ remediation under the condition of ensuring the safety of the soil environment. The inventor finds that the electric in-situ remediation can remove more than 75-90% of chromium from chromium-contaminated soil by carrying out electric in-situ remediation under the condition that the average water content of the contaminated soil is 10% to the saturated water holding capacity of the soil (the saturated water holding capacity of the soil is about 40-60%).
According to the invention, carbon dioxide gas is introduced into the chromium-polluted soil before and during the electric in-situ remediation, on one hand, the carbon dioxide gas has the functions of providing an anaerobic environment and protecting a desorbent from being biodegraded in the process of separating trivalent chromium, and on the other hand, after carbon dioxide is dissolved in water, the carbonate precipitate containing trivalent chromium can be partially dissolved, so that the separation of trivalent chromium is accelerated. In the actual operation process, the carbon dioxide inlet area is larger than the electric in-situ restoration area.
Injecting a sodium gluconate solution from a cathode well of the electrode, wherein under the action of an electric field, gluconate anions move to an electric field anode and meet cations containing trivalent chromium in the moving process to form an anion complex (shown as a formula (1)), then continuously moving to the electric field anode, and finally removing chromium pollutants in soil near the anode to realize soil remediation; after the remediation is finished, the residual sodium gluconate is removed by adding hydrogen peroxide into the remediated soil.
nC 6 H 11 O 7 - +Cr 3+ →(C 6 H 11 O 7 ) n Cr (n-3)- (n＞3) (1)
Experiments show that when the chromium-contaminated soil is electrically repaired in situ, the voltage applied between the electrodes is related to the water content of the soil, the unsaturated soil needs to be applied with higher voltage, and the saturated soil needs to be applied with lower voltage. In general, the voltage gradient of the electrodes is preferably controlled to be 2.0 to 4.0V/cm, preferably 3.0V/cm.
And when the chromium-contaminated soil reaches the remediation target, stopping adding the desorbent, stopping introducing carbon dioxide into the soil, and then injecting hydrogen peroxide into the soil after remediation is completed so as to effectively remove the residual desorbent in the soil.
The present invention has been tested to find that the desorbent must be selective for the target contaminant and not readily complexed with non-target cations (e.g., calcium or magnesium), and that the desorbent must be susceptible to oxidative degradation to avoid secondary soil contamination by the desorbent. The sodium gluconate screened by a large number of experiments can be used as a desorption agent to provide a ligand formed by gluconate and trivalent chromium-containing cations, and the ligand is separated from carbonate precipitates and the surfaces of soil particles and electrically removed. The tests carried out by the invention show that: by adopting the repairing method of the invention, more than 95% of chromium element can be removed at the anode of the electric field, but the effect is not achieved if other reagents such as sodium acetate or sodium citrate are used. The sodium gluconate can be quickly biodegraded under the condition that the soil is not protected by carbon dioxide, which is not beneficial to separating trivalent chromium, and the sodium gluconate is not obviously biodegraded before and during electric restoration. Experiments of the invention find that the sodium gluconate is easily oxidized and degraded by hydrogen peroxide, and the sodium gluconate is completely oxidized and degraded within 1 hour after the hydrogen peroxide with the concentration of 10 percent is introduced into the repaired soil, so that the secondary pollution of the soil is avoided.
The invention has the advantages and positive effects that:
(1) The invention provides a restoration method for desorbing trivalent chromium by using sodium gluconate protected by carbon dioxide for the first time, and the restoration method has high chromium pollution removal rate and high removal speed. According to the method for electrically repairing the chromium-contaminated soil in situ, sodium gluconate is preferably selected as a trivalent chromium desorption agent, the desorption agent is protected by carbon dioxide, and the precipitate containing trivalent chromium is partially dissolved, so that the chromium contamination removal rate is over 95% within 25 days after electrification and repair.
(2) Removing chromium pollution in situ and permanently restoring chromium-polluted soil. The electric in-situ remediation of the chromium-polluted soil by using the method has the advantages of high removal rate of chromium elements, no rebound phenomenon and realization of permanent remediation of chromium pollution.
(3) The soil structure is not damaged in the soil remediation process, and no secondary pollution is caused. In the process of electrically repairing chromium-contaminated soil in situ, the pH value, the soil structure and the water content of the soil are basically unchanged, and no residual desorbent exists after the desorbent is oxidized by introducing hydrogen peroxide after the repair is finished, so that no secondary pollution exists.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail with reference to the following embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
Example 1
Firstly, adjusting the water content of chromium-contaminated soil to be repaired to 10%, then respectively arranging a cathode well and an anode well of an electric system in the chromium-contaminated soil, and starting to repair the chromium-contaminated soil and soil outside the repair area by 0.1m before electrifying electrodes 3 Injecting carbon dioxide at a speed of/h, keeping the injection state of the carbon dioxide, and then injecting a sodium gluconate solution with the concentration of 0.01mol/L into the cathode well; and (3) switching on the two electrodes, controlling the voltage gradient to be 4.0V/cm, and detecting the total chromium content in the soil and calculating the chromium pollution removal rate respectively before and after 5, 15 and 25 days after the electrification. And after the restoration is finished, stopping injecting carbon dioxide, and injecting hydrogen peroxide with the concentration of 10% into the soil in the restoration area to oxidize and degrade the residual sodium gluconate.
Example 2
Firstly, adjusting the water content of the chromium-polluted soil to be repaired to 12%, then respectively arranging a cathode well and an anode well of an electric system in the chromium-polluted soil, and starting to move to the chromium-polluted soil repairing area and the soil outside the repairing area by 0.5m before the electrodes are electrified 3 Injecting carbon dioxide at a speed of/h, keeping the injection state of the carbon dioxide, and then injecting a sodium gluconate solution with the concentration of 0.05mol/L into the cathode well; connecting two electrodes, controlling voltage gradient at 3.0V/cm, and respectively powering on for 5, 15 and 25 daysAnd detecting the total chromium content in the soil and calculating the chromium pollution removal rate. And after the restoration is finished, stopping injecting carbon dioxide, and injecting hydrogen peroxide with the concentration of 10% into the soil of the restoration area to oxidize and degrade the residual sodium gluconate.
Example 3
Firstly, adjusting the water content of the chromium-polluted soil to be repaired to 40%, then respectively arranging a cathode well and an anode well of an electric system in the chromium-polluted soil, and starting to make the soil outside a chromium-polluted soil repair area and the repair area have a thickness of 1.0m before the electrodes are electrified 3 Injecting carbon dioxide at a speed of/h, keeping the injection state of the carbon dioxide, and then injecting a sodium gluconate solution with the concentration of 0.1mol/L into the cathode well; and (3) switching on the two electrodes, controlling the voltage gradient to be 2.0V/cm, and detecting the total chromium content in the soil and calculating the chromium pollution removal rate respectively before and after 5, 15 and 25 days after the electrification. And after the restoration is finished, stopping injecting carbon dioxide, and injecting hydrogen peroxide with the concentration of 10% into the soil in the restoration area to oxidize and degrade the residual sodium gluconate.
Comparative example 1
Firstly, adjusting the water content of the chromium-contaminated soil to be repaired to 12%, then respectively arranging a cathode well and an anode well of an electric system in the chromium-contaminated soil, and starting to fill 0.5m of the chromium-contaminated soil repair area and the soil outside the repair area before the electrodes are electrified 3 Injecting carbon dioxide at a speed of/h, keeping the injection state of the carbon dioxide, and then injecting a sodium citrate solution with the concentration of 0.1mol/L into a cathode well; and (3) switching on the two electrodes, controlling the voltage gradient to be 3.0V/cm, and detecting the total chromium content in the soil and calculating the chromium pollution removal rate respectively before and after 5, 15 and 25 days after the electrification. And after the restoration is finished, stopping injecting carbon dioxide, and injecting hydrogen peroxide with the concentration of 10% into the soil of the restoration area to oxidize and degrade the residual sodium citrate.
Comparative example 2
Firstly, adjusting the water content of the chromium-polluted soil to be repaired to 12%, then respectively arranging a cathode well and an anode well of an electric system in the chromium-polluted soil, and starting to move to the chromium-polluted soil repairing area and the soil outside the repairing area by 0.5m before the electrodes are electrified 3 Injecting carbon dioxide at a rate of/h, maintaining the injection of carbon dioxideInjecting sodium acetate solution with the concentration of 0.1mol/L into a cathode well; and (3) switching on the two electrodes, controlling the voltage gradient to be 3.0V/cm, and detecting the total chromium content in the soil and calculating the chromium pollution removal rate respectively before and after 5, 15 and 25 days after the electrification. And after the restoration is finished, stopping injecting carbon dioxide, and injecting hydrogen peroxide with the concentration of 10% into the soil of the restoration area to oxidize and degrade the residual sodium acetate.
Comparative example 3
The procedure and parameters were the same as in example 2 except that no carbon dioxide was introduced into the contaminated soil before and during energization.
Comparative example 4
The procedure and parameters were the same as in example 2 except that nitrogen was introduced into the contaminated soil before and during the energization.
In the soil polluted by chromium repaired by the methods of the above examples and comparative examples, the total chromium content in the soil is detected according to the method of HJ491-2009 flame atomic absorption spectrophotometry for detecting total chromium in the soil, and a soil sample is taken from the middle point of the two electrodes to detect the total chromium content; the chromium contamination removal rate = (total chromium content in soil before energization-total chromium content in soil after energization)/total chromium content in soil before energization × 100%, and the chromium contamination removal rate was calculated and the results are shown in table 1.
TABLE 1 chromium contamination removal Rate after electrification in each of the examples and comparative examples
Examples 1-3 in table 1 show that, by using the method for electrically repairing chromium-contaminated soil in situ provided by the invention, chromium contamination in contaminated soil after electrification can be rapidly and thoroughly removed, and the chromium contamination removal rate exceeds 95% after 25 days, wherein the effect of example 2 is the best.
From the comparison of example 2 with comparative example 1 and comparative example 2 in table 1, the results show that the preferred sodium gluconate of the present invention has a significant effect on the desorption and removal of chromium contamination as a trivalent chromium desorbent, while sodium citrate and sodium acetate have poor effect on the desorption of trivalent chromium.
Compared with the comparative example 3, the results of the example 2 in the table 1 show that the carbon dioxide is preferably introduced in the chromium-contaminated soil electrokinetic in-situ remediation process, and compared with the carbon dioxide which is not introduced in the chromium-contaminated soil electrokinetic in-situ remediation process, the carbon dioxide is not introduced in the chromium-contaminated soil electrokinetic in-situ remediation process, so that the desorption and removal of trivalent chromium in the contaminated soil are promoted.
From the comparison of example 2 with comparative example 4 in table 1, the results show that the preferred introduction of carbon dioxide into the chromium-contaminated soil according to the present invention has a certain dissolution effect on trivalent chromium in the precipitate containing trivalent chromium, while protecting the desorbent from degradation, compared to the introduction of nitrogen.
Finally, it should be noted that: the above examples are only intended to illustrate the technical solution of the present invention, and not to limit it; although the present invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: it is to be understood that modifications may be made to the technical solutions described in the foregoing embodiments, or some or all of the technical features may be equivalently replaced, and the modifications or the replacements may not make the essence of the corresponding technical solutions depart from the scope of the technical solutions of the embodiments of the present invention.
Claims (7)
1. An electric in-situ remediation method for chromium-contaminated soil is characterized by comprising the following steps: the method comprises the following steps:
s1, adjusting the water content of chromium-polluted soil to be more than 10% so that pore water between electrodes is electrically connected;
s2, introducing carbon dioxide gas into the chromium-contaminated soil, wherein the introduction rate of the carbon dioxide gas is 0.1-1.0m 3 Providing an anaerobic environment and reducing biodegradation of sodium gluconate; after carbon dioxide is dissolved in water, carbonate precipitate containing trivalent chromium can be partially dissolved, and separation of trivalent chromium is accelerated;
s3, adding the sodium gluconate solution into an electric remediation cathode well of the chromium-contaminated soil; the concentration of the sodium gluconate solution is 0.01-0.1mol/L;
s4, applying direct current to the two electrodes arranged in the chromium-polluted soil area to electrically repair the chromium-polluted soil in situ; under the action of an electric field, the gluconate ions migrate to the anode and form a ligand with trivalent chromium-containing cations in the migration process, and the trivalent chromium is separated from insoluble precipitates or the surface of soil particles, so that the chromium in the soil polluted by the chromium is removed;
and S5, stopping introducing carbon dioxide gas after the chromium-polluted soil reaches the remediation target, adding hydrogen peroxide into the remediated soil, and removing redundant sodium gluconate.
2. The electrokinetic in-situ remediation method of chromium-contaminated soil according to claim 1, characterized in that: in the step S1, the water content of the chromium-polluted soil is adjusted to be more than 12%.
3. The electrokinetic in-situ remediation method of chromium-contaminated soil according to claim 1, characterized in that: the carbon dioxide gas introduction rate is 0.5m 3 /h。
4. The method for electrokinetic in-situ remediation of chromium-contaminated soil according to claim 1, characterized in that: the concentration of the sodium gluconate solution is 0.05mol/L.
5. The method for electrokinetic in-situ remediation of chromium-contaminated soil according to claim 1, characterized in that: in the step S4, the voltage gradient between the two electrodes is controlled to be 2.0-4.0V/cm.
6. The method for electrokinetic in-situ remediation of chromium-contaminated soil according to claim 5, characterized in that: the voltage gradient between the two electrodes was controlled at 3.0V/cm.
7. The method for electrokinetic in-situ remediation of chromium-contaminated soil according to claim 1, characterized in that: in the step S5, the concentration of the hydrogen peroxide is 10%.
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