CN109304365B - Electric remediation method for antimony-polluted soil - Google Patents

Electric remediation method for antimony-polluted soil Download PDF

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CN109304365B
CN109304365B CN201811465245.6A CN201811465245A CN109304365B CN 109304365 B CN109304365 B CN 109304365B CN 201811465245 A CN201811465245 A CN 201811465245A CN 109304365 B CN109304365 B CN 109304365B
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antimony
groove
filter paper
stainless steel
plate
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CN109304365A (en
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汪一潭
秦丰林
郑伟
张慧
任欢鱼
刘新荣
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Nanjing Ditian High Tech Industrial Technology Research Institute Co ltd
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Nanjing Ditian High Tech Industrial Technology Research Institute Co ltd
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B09DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
    • B09CRECLAMATION OF CONTAMINATED SOIL
    • B09C1/00Reclamation of contaminated soil
    • B09C1/08Reclamation of contaminated soil chemically
    • B09C1/085Reclamation of contaminated soil chemically electrochemically, e.g. by electrokinetics

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  • Chemical Kinetics & Catalysis (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Soil Sciences (AREA)
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  • Environmental & Geological Engineering (AREA)
  • Water Treatment By Electricity Or Magnetism (AREA)
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Abstract

The invention discloses an electric repair method for antimony-polluted soil, which is characterized in that pentavalent antimony is reduced to trivalent antimony in a cathode through the synergistic action of ferrous ions and phosphate ions of the cathode in an electric repair reactor, and the trivalent antimony and the ferrous ions are purified and removed through coprecipitation or flocculation; the technical scheme of the invention has the following beneficial effects: the working solution formula is simple in raw materials, good in treatment effect, high in repair speed and simple and convenient to operate, is applied to electric repair of antimony-polluted soil, improves the repair efficiency of the antimony-polluted soil by 50% -100%, and accelerates the repair speed.

Description

Electric remediation method for antimony-polluted soil
Technical Field
The invention relates to the technical field of soil remediation, in particular to an electric remediation method for antimony-polluted soil.
Background
Antimony is not a naturally abundant element and is present in the bottom shell in an amount of approximately 0.2mg/kg, but the global flux of antimony has increased at least 10-fold in the last decade due to the rise in environmental antimony concentrations caused by human activity. The collected hair of residents in polluted areas has an antimony content of 15.9 mg/kg, so that a cleaning technology must be developed and effectively implemented in mining areas to remove antimony from soil.
The existing technologies for treating antimony-polluted soil mainly comprise phytoremediation, microbial remediation and leaching. The operation cost of phytoremediation is low, and the recovery and treatment of enriched heavy metals are easy; however, the time is long, the molecular, biochemical and physiological processes of antimony absorption by hyper-accumulative plants are deeply clarified only aiming at antimony in shallow underground water, surface soil and sediments, the potential exertion of phytoremediation is limited, the feeding behavior of phytoremediation in herbivorous places enables antimony to enter a food chain, the problem of post-treatment of phytoremediation is difficult to solve, and external plant species may have adverse effects on local soil and biodiversity. Although the microbial remediation technology has little influence on the environment, secondary pollution can not be caused; however, the time consumption is long, the conditions are harsh, not all pollutants entering the environment can be biologically utilized, and specific organisms generally can only absorb, utilize, degrade and convert specific types of chemical substances. The cleaning solution for the soil leaching technology is various in types, can be recycled and can also be used for removing residual pollutants by injecting underground water for multiple times, but the underground water is polluted to a certain extent due to improper treatment, so that secondary pollution is caused.
Electrokinetic remediation is a technique for in situ remediation of contaminated soil by vertically placing appropriate anodes and cathodes underground and applying a low power dc electric field to remove contaminants from the soil. The electric restoration has the advantages of wide applicability, high energy efficiency, easy automatic operation, environmental friendliness, low cost and the like. The successful case of electrically repairing soil pollution exists, and various strengthening technologies for soil repair are reported in documents. There have been no reports and successful cases of using electrokinetic remediation techniques to remediate antimony contaminated soil.
Disclosure of Invention
Aiming at the problems, the invention aims to provide an electric repair method for antimony-polluted soil, and particularly provides a working solution formula which is simple in raw material, good in treatment effect, high in repair speed and simple and convenient to operate, and is applied to electric repair of antimony-polluted soil, so that the repair efficiency of the antimony-polluted soil is improved by 50% -100%, and the repair speed is increased.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
the working solution formula for electrically repairing antimony-polluted soil comprises an anode working solution and a cathode buffer solution, wherein the anode working solution is a potassium dihydrogen phosphate-potassium hydroxide aqueous solution which is 0.05-0.5 mol/L and prepared from potassium dihydrogen phosphate and potassium hydroxide according to the mass concentration ratio of 1:1, and the cathode buffer solution is a potassium acetate-acetic acid aqueous solution which is 0.2-0.8 mol/L and prepared from potassium acetate and acetic acid according to the mass concentration ratio of 1-2: 1-2.
Preferably, the concentration range of the anode working solution is 0.05-0.5 mol/L.
Preferably, the concentration range of the cathode buffer solution is 0.2-0.8 mol/L.
Preferably, the content of the monopotassium phosphate is more than or equal to 99 percent; potassium hydroxide with the content more than or equal to 99 percent; potassium acetate, the content of which is more than or equal to 99 percent; the concentration of the acetic acid is 36% -38%.
The application of the working solution formula for electrokinetic remediation of antimony-contaminated soil comprises the following steps:
step 1: collecting soil to be restored, filling the soil to be restored into a reactor in an electric restoration device, and adopting an iron plate as an anode plate and a steel plate as a cathode plate;
step 2: an anode tank and a cathode tank are respectively arranged on two sides of the reactor, and anode working solution and cathode buffer solution are respectively filled in the anode tank and the cathode tank;
and step 3: adjusting the current density to 1-15 mA/cm2The ratio of the area of the polar plate to the area of the side face of the reactor is 1/2-1/4 m2/m2The distance between the polar plates is 15-25 cm, a direct-current power supply is adopted for intermittent power supply, and the power is cut off for 2-4 hours after 2-4 hours of power supply and is continuously maintained;
and 4, step 4: sampling every 2h to measure the pH value of the working solution, ensuring that the pH value is between 4.5 and 9, and stopping power supply after 72 h;
and 5: the pentavalent antimony is reduced to trivalent antimony in the cathode and purified and removed by coprecipitation or flocculation with ferrous ions. Preferably, the reactor both ends of electronic prosthetic devices still all set up stainless steel rack, and can dismantle in the stainless steel rack and set up filter paper, filter paper passes through docking mechanism butt joint chucking, the stainless steel rack is square structure, includes middle check wire compartment and establishes the filter paper groove on middle check wire compartment both sides open the groove that link up that is used for liquid to pass through in the side of stainless steel rack, link up the groove follow one side intercommunication to the opposite side of stainless steel rack.
Preferably, the bottom of the middle grid groove is provided with a conical positioning groove, and a stainless steel grid is correspondingly arranged in the middle grid groove.
Preferably, the butting mechanism is composed of two spring steel plates which are arranged oppositely, the top of each spring steel plate is fixed on the inner wall of the filter paper groove, the lower end of each spring steel plate is an integrally formed inclined butting part, and a filter paper channel for installing filter paper is formed between the inclined butting parts on the two spring steel plates.
As preferred still be equipped with on the stainless steel rack and be used for right spring steel plate carries out the locking mechanism who locks, locking mechanism transversely sets up on the filter paper groove, and include locking bolt and the locking post of welding at locking bolt tip, locking post terminal surface is the wedge structure, every all opened the locking groove on spring steel plate's the lateral surface, the wedge structure corresponds locking groove controls two spring steel plate motion in opposite directions through adjusting locking bolt, further realizes the tight operation of clamp to filter paper.
Preferably, a layer of magnetic plate is further fixed on the end face of the wedge-shaped structure, a magnetic sheet is tightly connected in the locking groove, and the magnetic plate and the magnetic sheet attract each other.
The invention has the beneficial effects that:
firstly: the method has the advantages that the ion exchange capacity and the adsorption capacity are improved, the migration capacity of antimony in the soil can be improved, the removal rate of antimony in the soil is improved, and the removal rate is improved by 50% -100%;
secondly, the method comprises the following steps: the use of the potassium dihydrogen phosphate-potassium hydroxide solution increases the phosphorus content of the soil, and provides advantages for the soil as farmland soil; because potassium acetate-acetic acid is used as a buffer solution, the probability of forming insoluble sodium antimonate is reduced, the removal rate of antimony is improved by 50-100%, and the electric repair work efficiency is increased by 1.5-2 times.
Drawings
Fig. 1 is a schematic view of an electromotive prosthetic device of the present invention.
Fig. 2 is a schematic view of a stainless steel wire frame of the present invention.
Fig. 3 is a front view schematically showing the stainless steel net rack of the present invention.
Fig. 4 is an enlarged view of a portion D in fig. 3.
Fig. 5 is a side view of the stainless steel wire frame of the present invention.
Fig. 6 is a schematic view of a stainless steel mesh.
Wherein: 1-reactor, 2-anode tank, 3-cathode tank, 4-anode plate, 5-cathode plate, 6-anode working solution, 7-cathode buffer solution, 8-gas outlet and detection hole, 9-stainless steel net frame, 10-middle grid tank, 101-conical positioning groove, 11-paper filtering tank, 12-through tank, 13-spring steel plate, 131-inclined butt joint part, 14-locking bolt, 15-locking column, 16-wedge structure, 17-locking tank, 18-polluted soil, 19-direct current power supply, 20-ammeter, 21-conical clamping end and 22-stainless steel grid.
Detailed Description
In order to make those skilled in the art better understand the technical solution of the present invention, the following further describes the technical solution of the present invention with reference to the drawings and the embodiments.
A working solution formula for electrically repairing antimony-polluted soil 18 comprises an anode working solution 6 and a cathode buffer solution 7, wherein the anode working solution 6 is a potassium dihydrogen phosphate-potassium hydroxide aqueous solution which is prepared from potassium dihydrogen phosphate and potassium hydroxide according to a mass concentration ratio of 1:1 and has a concentration of 0.05-0.5 mol/L, and the cathode buffer solution 7 is a potassium acetate-acetic acid aqueous solution which is prepared from potassium acetate and acetic acid according to a mass concentration ratio of 1-2: 1-2 and has a concentration of 0.2-0.8 mol/L; the concentration range of the anode working solution 6 is 0.05-0.5 mol/L, and the concentration range of the cathode buffer solution 7 is 0.2-0.8 mol/L; the content of the monopotassium phosphate is more than or equal to 99 percent, and the content specifically refers to mass concentration; the content of the potassium hydroxide is more than or equal to 99 percent, and the content specifically refers to mass concentration; potassium acetate, the content of which is more than or equal to 99 percent, the content specifically refers to mass concentration; the concentration of the acetic acid is 36% -38%.
Referring to the attached figures 1-6, the application of the working solution formula for electrokinetic remediation of antimony-contaminated soil 18 comprises the following steps:
step 1: collecting soil to be restored, filling the soil to be restored into a reactor 1 in an electric restoration device, and adopting an iron plate as an anode plate 4 and a steel plate as a cathode plate 5;
step 2: an anode tank 2 and a cathode tank 3 are respectively arranged at two sides of the reactor 1, an anode working solution 6 and a cathode buffer solution 7 are respectively filled in the anode tank 2 and the cathode tank 3, and gas outlet and detection holes 8 are respectively arranged on the anode tank 2 and the cathode tank 3; the stainless steel grid 22 and the filter paper are needed in the actual electrolysis operation, but the existing stainless steel grid 22 cannot be disassembled and is not convenient to install, and the filter paper is directly placed on the side surface of the stainless steel grid 22, so that the filter paper is light and is not easy to well tile in the filtering process, and the filter paper is easy to bend when vertically arranged, thereby losing the filtering effect and further influencing the efficiency and effect of replacement of working solution and buffer solution with antimony in soil in the electrolysis process, therefore, the invention improves the installation structure of the stainless steel grid 22 and the filter paper;
the reactor 1 of the electric repairing device is characterized in that stainless steel net racks 9 are arranged at two ends of the reactor 1, filter paper is detachably arranged in the stainless steel net racks 9 and is butted and clamped through a butting mechanism, each stainless steel net rack 9 is of a square structure and comprises a middle grid groove 10 and filter paper grooves 11 arranged at two sides of the middle grid groove 10, a through groove 12 for liquid to pass through is formed in the side surface of each stainless steel net rack 9, the through groove 12 is communicated from one side of the stainless steel net rack 9 to the other side, after the stainless steel grid 22 and the filter paper are installed in the electrolytic process, the liquid in the electrolytic process passes through the through groove 12, and the filter paper and the stainless steel grid 22 are arranged in the through groove 12; the bottom of the middle grid groove 10 is provided with a conical positioning groove 101, a stainless steel grid 22 is correspondingly installed in the middle grid groove 10, when the stainless steel grid 22 is installed, the bottom of the stainless steel grid 22 is provided with a conical clamping end 21, the conical clamping end 21 is correspondingly clamped with the cylindrical positioning groove at the bottom of the middle grid groove 10, and two ends of the middle grid groove 10 are also provided with closed ends to avoid liquid leakage;
the butt joint mechanism is composed of two spring steel plates 13 which are arranged oppositely, the top of each spring steel plate 13 is fixed on the inner wall of the filter paper groove 11, and the lower end is an integrally formed inclined butt-joint part 131, a filter paper channel for installing filter paper is formed between the inclined butt-joint parts 131 on the two spring steel plates 13, the stainless steel net rack 9 is also provided with a locking mechanism for locking the spring steel plate 13, the locking mechanism is transversely arranged on the filter paper slot 11, and comprises a locking bolt 14 and a locking column 15 welded at the end of the locking bolt 14, the end surface of the locking column 15 is a wedge-shaped structure 16, the outer side surface of each spring steel plate 13 is provided with a locking groove 17, the wedge-shaped structure 16 corresponds to the locking groove 17, the locking bolt 14 is adjusted to control the two spring steel plates 13 to move oppositely, so that the filter paper is further clamped; the top end of the filter paper groove 11 is provided with a small opening, in order to set a spring steel plate 13, the spring steel plate 13 can be fixed on the inner wall of the filter paper groove 11 through rivets and the like, two side edges of the filter paper groove 11 are respectively provided with a threaded hole in opposite directions, a locking bolt 14 is arranged in the threaded hole, a filter paper channel formed by the spring steel plate 13 is firstly enlarged in the operation process, the filter paper is vertically and carefully placed in, the bottom of the filter paper is clamped through a slotted hole on a square groove before the filter paper is placed in, the bottom of the filter paper is clamped in the square groove, then the holes of the two spring steel plates 13 in the filter paper groove 11 are opened, the filter paper with the square groove is placed in the filter paper until the bottom of the square groove is just placed in the bottom of the filter paper groove 11, the height of the filter paper is slightly higher than that of the filter paper groove 11, then the locking bolt 14 is adjusted, a wedge-shaped structure 16 at the end part of the locking column 15 corresponds to a locking groove 17 at the side surface of the spring steel plate 13, thereby driving the two spring steel plates 13 to approach and clamp the upper end of the filter paper;
further, a layer of magnetic plate is fixed on the end face of the wedge-shaped structure 16, a magnetic sheet is tightly connected in the locking groove 17, and the magnetic plate and the magnetic sheet are attracted; the magnetic plate and the magnetic attraction piece are arranged, namely, the magnetic plate and the magnetic attraction piece in the locking groove 17 can be further used for driving the spring steel plate 13 to move outwards in the process that the locking bolt 14 rotates outwards through the attraction effect of the magnetic piece and the magnetic plate in the locking groove 17 when a hole between the two spring steel plates 13 is opened, and then the spring steel plates are opened and filter paper is to be placed in;
and step 3: adjusting the current density to 1-15 mA/cm2The ratio of the area of the polar plate to the area of the side surface of the reactor 1 is 1/2-1/4 m2/m2The distance between the polar plates is 15-25 cm, a direct current power supply 19 is adopted for intermittent power supply for 2-4 hPowering off for 2-4 h after power is on, and continuously;
and 4, step 4: sampling every 2h to measure the pH value of the working solution, ensuring that the pH value is between 4.5 and 9, and stopping power supply after 72 h;
and 5: the pentavalent antimony is reduced to trivalent antimony in the cathode and purified and removed by coprecipitation or flocculation with ferrous ions.
In the electric repairing device, an iron plate is arranged as an anode plate, a steel plate is arranged as a cathode plate, antimony-polluted soil 18 is filled in a reactor 1, stainless steel nets and filter paper are added at two ends of the reactor 1, a cathode tank 3 and an anode tank 2 are externally connected, the steel plate and the iron plate are respectively connected at the outer ends of the cathode tank 3 and the anode tank 2, and a power supply and an ammeter 20 are connected between the two electrodes. Adding a potassium dihydrogen phosphate-potassium hydroxide solution into the anode tank 2; adding a buffer solution into the cathode tank 3;
in the electric repair reactor 1, through the synergistic effect of ferrous ions and phosphate ions of the anode, original free antimony is transferred to the cathode in an electromigration mode, electrons lost by the anode are reduced to trivalent antimony, and the trivalent antimony is purified and removed through coprecipitation or flocculation with ferrous ions generated after electrochemical dissolution of the anode potential.
Example 1
Preparing a 1:1 0.05mol/L potassium dihydrogen phosphate-potassium hydroxide solution and a 1:1 0.2mol/L buffer solution. In the electric repairing reaction device, the iron plate is used as an anode, the steel plate is used as a cathode, a direct current power supply is adopted for regular discontinuous power supply, and the current density is 1mA/cm2The ratio of the area of the plate to the area of the side surface of the reactor is 1/2 m2/m2The distance between the polar plates is 15 cm. 0.05mol/L potassium dihydrogen phosphate-potassium hydroxide solution is added into the anode tank, 0.1mol/L buffer solution is added into the cathode tank, the adding mode is one-time adding, and samples are taken every 2 h. And (3) switching on a direct current power supply, powering off for 2h after 2h, and stopping power supply after 72h, wherein the removal rate of the antimony in the soil reaches 30 percent.
Example 2
Preparing a 1:1 0.5mol/L potassium dihydrogen phosphate-potassium hydroxide solution and a 1:1 0.8mol/L buffer solution. In the electric repairing reaction device, the iron plate isThe anode and the steel plate are used as the cathode, a direct current power supply is adopted for regular discontinuous power supply, and the current density is 1mA/cm2The ratio of the area of the plate to the area of the side surface of the reactor is 1/2 m2/m2The distance between the polar plates is 15 cm. 0.5mol/L potassium dihydrogen phosphate-potassium hydroxide solution is added into the anode tank, 0.8mol/L buffer solution is added into the cathode tank, the adding mode is one-time adding, and samples are taken every 2 h. And (3) switching on a direct current power supply, powering off for 2h after 2h, and stopping power supply after 72h, wherein the removal rate of the antimony in the soil reaches 41 percent.
Example 3
Preparing a 1:1 0.5mol/L potassium dihydrogen phosphate-potassium hydroxide solution and a 1:1 0.8mol/L buffer solution. In the electric repairing reactor, iron plate as anode and steel plate as cathode are powered intermittently with DC power supply in current density of 15mA/cm2The ratio of the area of the plate to the area of the side surface of the reactor is 1/2 m2/m2And the distance between the polar plates is 25 cm. 0.5mol/L potassium dihydrogen phosphate-potassium hydroxide solution is added into the anode tank, 0.8mol/L buffer solution is added into the cathode tank, the adding mode is one-time adding, and samples are taken every 2 h. And (3) switching on a direct current power supply, powering off for 4h after 4h, and stopping power supply after 72h, wherein the removal rate of the antimony in the soil reaches 50.9 percent.
The following table is a comparison table of the concentration of antimony in soil and the concentration of antimony in raw soil after remediation according to examples 1-3
Figure DEST_PATH_IMAGE001
The foregoing shows and describes the general principles, essential features, and advantages of the invention. It will be understood by those skilled in the art that the present invention is not limited to the embodiments described above, which are described in the specification and illustrated only to illustrate the principle of the present invention, but that various changes and modifications may be made therein without departing from the spirit and scope of the present invention, which fall within the scope of the invention as claimed. The scope of the invention is defined by the appended claims and equivalents thereof.

Claims (5)

1. An electric restoration method for antimony-polluted soil is characterized by comprising the following steps: the method comprises the following steps:
step 1: collecting soil to be restored, filling the soil to be restored into a reactor in an electric restoration device, and adopting an iron plate as an anode plate and a steel plate as a cathode plate;
step 2: an anode tank and a cathode tank are respectively arranged on two sides of the reactor, and anode working solution and cathode buffer solution are respectively filled in the anode tank and the cathode tank;
and step 3: adjusting the current density to 1-15 mA/cm2The ratio of the area of the polar plate to the area of the side face of the reactor is 1/2-1/4 m2/m2The distance between the polar plates is 15-25 cm, a direct-current power supply is adopted for intermittent power supply, and the power is cut off for 2-4 hours after 2-4 hours of power supply and is continuously maintained;
and 4, step 4: sampling every 2h to measure the pH value of the working solution, ensuring that the pH value is between 4.5 and 9, and stopping power supply after 72 h;
and 5: the pentavalent antimony is reduced into trivalent antimony in the cathode, and is purified and removed through coprecipitation or flocculation with ferrous ions;
wherein:
in the electric repairing device in the step 1, stainless steel net racks are arranged at two ends of a reactor, filter paper is detachably arranged in the stainless steel net racks, and the filter paper is butted and clamped through a butting mechanism; the stainless steel net rack is of a square structure and comprises a middle grid groove and filter paper grooves arranged on two sides of the middle grid groove, a through groove for liquid to pass through is formed in the side face of the stainless steel net rack, and the through groove is communicated from one side of the stainless steel net rack to the other side of the stainless steel net rack; the bottom of the middle grid groove is provided with a conical positioning groove, and a stainless steel grid is correspondingly arranged in the middle grid groove;
the butt joint mechanism is composed of two spring steel plates which are arranged oppositely, the top of each spring steel plate is fixed on the inner wall of the filter paper groove, the lower end of each spring steel plate is an integrally formed inclined butt joint part, and a filter paper channel for installing filter paper is formed between the inclined butt joint parts on the two spring steel plates;
the stainless steel net rack is also provided with a locking mechanism for locking the spring steel plate;
the locking mechanism is transversely arranged on the filter paper groove and comprises a locking bolt and a locking column welded at the end part of the locking bolt;
the end face of the locking column is of a wedge-shaped structure, and a locking groove is formed in the outer side face of each spring steel plate; the wedge-shaped structure corresponds to the locking groove, and the two spring steel plates are controlled to move oppositely by adjusting the locking bolt, so that the filter paper is further clamped.
2. The method for electrically remediating antimony-contaminated soil as claimed in claim 1, wherein: the anode working solution is a potassium dihydrogen phosphate-potassium hydroxide aqueous solution which is prepared from potassium dihydrogen phosphate and potassium hydroxide according to the mass concentration ratio of 1:1 and has a mass concentration of 0.05-0.5 mol/L.
3. The method for electrically remediating antimony-contaminated soil as claimed in claim 2, wherein: the cathode buffer solution is a potassium acetate-acetic acid aqueous solution which is prepared from potassium acetate and acetic acid according to the mass concentration of 1-2: 1-2 and has a concentration of 0.2-0.8 mol/L.
4. The method for electrically remediating antimony-contaminated soil as claimed in claim 3, wherein: the content of the monopotassium phosphate is more than or equal to 99 percent; potassium hydroxide with the content more than or equal to 99 percent; potassium acetate, the content of which is more than or equal to 99 percent; the concentration of the acetic acid is 36% -38%.
5. The method for electrically restoring the antimony-polluted soil as claimed in claim 1, wherein a magnetic plate is further fixed to an end face of the wedge-shaped structure, a magnetic sheet is tightly connected in the locking groove, and the magnetic plate and the magnetic sheet are attracted to each other.
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CN104724797B (en) * 2014-12-16 2017-12-08 中国科学院生态环境研究中心 A kind of manganese ion strengthens the method that electrochemistry removes quinquevalence antimony pollutant in water removal
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Denomination of invention: An electric remediation method for antimony contaminated soil

Effective date of registration: 20211118

Granted publication date: 20210928

Pledgee: China Construction Bank Corporation Nanjing Jiangbei new area branch

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