CN109848201B - Electric power driving and electrothermal activation oxidation/reduction repair method - Google Patents
Electric power driving and electrothermal activation oxidation/reduction repair method Download PDFInfo
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Abstract
The invention discloses an electric power driving and electrothermal activation oxidation/reduction repairing method, which comprises the following steps: injecting an oxidation/reduction agent into the soil to be treated; inserting a cathode and an anode which are connected with a power supply into soil to be treated respectively, electrifying to form an electric field, and driving an oxidation/reduction agent to be transmitted in the soil by electric power; the heating and the temperature rise are realized through electric heating activation, and the oxidizing agent can be activated after the temperature rises, so that the soil remediation is realized; the electric heating activation is to add strong electrolyte into the soil to be treated. The invention utilizes the heat generated by the electrokinetic process to activate the oxidation agent by a regulation and control means, can obviously improve the oxidation capacity and the repair efficiency, does not introduce other exogenous substances, has simple and easy operation, realizes the practical application of the electrokinetic repair technology, enhances the in-situ mass transfer capacity of the chemical oxidation method, achieves three purposes by one, has high efficiency, practicability and strong engineering operability, and is an efficient repair technology with great application prospect.
Description
Technical Field
The invention relates to the technical field of soil pollution treatment, in particular to an electric power driving and electrothermal activation oxidation/reduction repairing method.
Background
Chemical oxidation/reduction is the most common method for remediating organically-contaminated soils. In-situ chemical oxidation/reduction is the injection of an oxidizing/reducing agent into the underground environment to convert toxic and harmful pollutants into non-toxic and harmless or low-toxicity and stable substances. The main advantage of the method is that the advanced oxidation reaction mainly based on free radical reaction can degrade the organic matters almost indiscriminately, and the organic matters can be completely mineralized into CO as long as the conditions are proper2、H2O and inorganic ions, which is a relatively thorough repair technology. However, the repairing effect of the technology in the viscous soil is greatly reduced, mainly because the viscous soil has small pores and poor permeability, the mass transfer of the medicament in the soil is greatly limited, and the medicament cannot be effectively contacted with pollutants. This has become an important technical problem that restricts the remediation of the viscous contaminated soil. At present, the mass transfer is enhanced by increasing the pressure to enable the soil to form cracks, but the secondary cracks are usually uneven and larger cracks, a mass transfer preferential channel can be formed, solution short flow is caused, although the diffusion radius is increased, the oxidizing agent cannot be in microcosmic uniform contact with soil pollutants, and the improvement effect is limited. Another approach is to reduce the injector well placement radius but increase the number of injectors resulting in increased capital investment.
The electric power driving solution is transmitted in the field, the oxidation/reduction agent is driven to enter the soil by the electric power to react with the polluted contact, the problem of long-distance transmission of the oxidant solution in the viscous soil can be easily realized, and the engineering application of the technology becomes very feasible.
Persulfate is a commonly used oxidant, but the single use of persulfate has low efficiency and needs to exert stronger oxidation under the condition of activation, and commonly used activation technologies comprise heating, alkali, ultraviolet light, ultrasound, microwave, metal, activated carbon, organic matters and H2O2And the like. Among them, the thermal activation technology only needs to regulate the temperature of the system, and does not introduce other substances, and is considered as a clean in-situ repair technology. But thermal activation cannot be realized in a polluted site, and the application field of the thermal activation is limited.
Disclosure of Invention
The present invention aims at providing an electromotive force driving and electrothermal activation oxidation/reduction repairing method to solve the above-mentioned defects of the background art.
The invention is realized by the following technical scheme:
an electric power driving and electrothermal activation oxidation/reduction repairing method comprises the following steps:
injecting an oxidation/reduction agent into soil to be treated;
inserting a cathode and an anode connected with a power supply into the soil to be treated respectively, electrifying to form an electric field, and driving the oxidation/reduction agent to be transmitted in the soil by electric power;
thirdly, through electric heating activation, charged ions in the system move and collide with each other to convert electric energy into heat energy, heating and temperature rise are realized, and the oxidizing agent can be activated after the temperature rises, so that soil remediation is realized;
the electric heating activation is to add strong electrolyte into the soil to be treated.
Preferably, the acidity of the soil to be treated should be controlled to be between 3 and 8.
Preferably, in the second step, the electric drive is in a constant voltage or constant current mode. Adopting a constant voltage mode, and setting the voltage gradient at 0-5V/cm; by constant current, the electric field density is set at 0-1A/cm2。
The strong electrolyte refers to an electrolyte which completely ionizes ions in an aqueous solution or a molten state. As a preferred technical solution, the strong electrolyte is selected from at least one of sodium chloride and potassium chloride.
Preferably, the strong electrolyte is added in the form of aqueous solution, and the introduction of the strong electrolyte adopts two modes of electric power transmission and injection.
Further preferably, the molar ratio between the oxidant and the strong electrolyte is 1: 1-5. The strong electrolyte can be injected separately or together with the oxidant.
As a further preferred technical solution, the electro-thermal activation further comprises electrode switching.
The switching frequency of the electrode switching is once in 6-12 hours.
The purpose of heating and temperature rising is realized by the power supply regulation and control means, the temperature can rise to 100 ℃, and persulfate and other oxidizing agents can be activated after the temperature rises, so that the reaction capacity is enhanced, and the pollutant degradation rate is improved.
The method for repairing the target pollutants through the electric power driving and the electric heating activation oxidation/reduction is realized by regulating and controlling the proportion of the total energy consumption, the heat effect energy consumption of the total energy consumption, the invalid substance migration energy consumption and the target pollutants removal energy consumption in the electric power process, and the energy distribution can be changed to the direction beneficial to improving the target pollutants removal rate by setting a proper voltage gradient, properly acidifying the soil to be tested, introducing proper working solution, an optimizing device and other measures and the like, so that the benefit of the whole repairing engineering is improved; in turn, the electric energy loss proportion is biased to heat effect energy consumption through the regulation and control of the means, and then dual functions of driving pollutants and heating soil are achieved.
In the invention, the introduction of the strong electrolyte for soil acidification can realize the violent rise of system current, thereby realizing the rapid conversion of electric energy into heat energy. However, excessive acidification and excessive introduction of strong electrolyte can cause local high conductivity phenomenon to induce ion motion traps, and the current of the system is rapidly reduced after being violently increased, so that insufficient heat generation is caused. Moreover, the present invention is primarily directed toThe organic pollutants are generally not charged, the movement in the system mainly depends on electroosmotic flow, and the oxidant is not suitable for being combined with OH-The reaction takes place to form a precipitate, and the soil pH of the present invention is controlled to be between 3 and 8.
The introduction of the strong electrolyte mainly considers that the introduced electrolyte cannot cause negative influence on the oxidation-reduction reaction and cannot form precipitates with metal ions in a system. If the electrolyte is introduced and metal ions in the system are easy to form precipitates, the precipitates can not only block the soil pores and prevent pollutants from moving and contacting with an oxidizing agent or a reducing agent, but also cause the local resistance to be increased sharply, and the current of the whole system is reduced rapidly. Practice has shown that the high current in the present invention has a significant impact on heat generation compared to high resistance. The system generates weak heat at low current and high resistance, and is not enough to realize the action of activation reaction. Thus, the strong electrolyte anion introduced in the present invention is typically Cl-The cation is typically Na+、K+. The introduction of strong electrolyte is mainly carried out by two modes of injection and automatic transmission of electric power. The electric power transmission mainly introduces electrolyte into an electrode tank and enters soil through electric field driving; the manual injection is mainly based on the requirement of different point locations on the electrolyte, and the fixed-point injection is carried out.
The invention mainly uses a constant voltage mode for regulating and controlling the power supply. Practice proves that the constant current mode is more beneficial to quick temperature rise of soil and timely temperature regulation, but the voltage between electrodes under the constant current is continuously raised, so that great unsafe factors are caused, and the method is not suitable for engineering application. Generally, the system is heated by using a direct current artificial frequency conversion mode, and a heating area is regulated and controlled.
In the invention, the electrolyte is continuously consumed in the electrochemical reaction of the electrode, so that the concentration of charged ions of the system is reduced, and the current is continuously weakened. The invention mainly realizes that the body system maintains a higher current by a method of continuously introducing strong electrolyte solution. The invention uses the electrode approach method to realize the special enhancement of the fixed-point area and weaken a series of negative effects caused by focusing effect and the like. Any way of constructing the electrode matrix on the premise of adopting the concept of the invention belongs to the protection scope of the patent. It is to be noted that the introduction of the strong electrolyte in the present invention must be performed by means of an aqueous electrolyte solution. The continuous volatilization of the moisture due to the temperature rise of the soil and the continuous supplement of the moisture are also the main contents for realizing the invention.
The relation among voltage, current and resistance in the system is different from the classical ohm law, and the resistance suffered by a single charged ion is increased while the current of the system is increased by introducing the strong electrolyte. Thus, to consume more energy for heat generation, only a sufficient amount of electrolyte needs to be added. The amount of electrolyte should not be too high to affect the transport of the oxidant. The electrolyte may be injected separately or co-injected with the oxidant. Typically, the concentration ratio between oxidant and incoming electrolyte is between 1 and 5 times to achieve a balance between high heat generation and oxidant mass transfer requirements. The specific requirements are respectively adjusted according to soil property, pollutant type and oxidant type. The specific ratios are not limited to the general parameters provided by the present invention.
The electrode conversion and the introduction of strong electrolyte belong to the means of regulating and controlling temperature rise. The transformation with the electrodes can release part of deposited electrolyte in the soil again, so that the system current is increased and the temperature is increased; meanwhile, the pollutant and the oxidant can be driven to do reciprocating motion in the soil, and the effects of homogenizing a reaction system and increasing reaction contact can be achieved. In addition, the electrode switching also acts to make the temperature distribution between the two electrodes more uniform. According to practice, the invention relates to an electrode switching frequency which is preferably once, typically in the range of 6 to 12 hours. The specific requirements are respectively adjusted according to soil property, pollutant type and oxidant type. The specific frequency is not limited to the general parameters provided by the present invention.
The oxidizing agent comprises hydrogen peroxide, Fenton (fenton) reagent (ferrous ions are used as a catalyst, and hydrogen peroxide is used for chemical oxidation to generate hydroxyl free radicals with strong oxidizing property, organic free radicals are generated with refractory organic matters in aqueous solution to cause the structure of the hydroxyl free radicals to be damaged and finally oxidized and decomposed), Fenton-like reagent, persulfate (such as sodium persulfate solution), permanganate (such as potassium permanganate aqueous solution) and the like, and the reducing agent comprises an iron-based reducing agent (such as zero-valent iron and ferrous ions), sulfide, sulfite and the like.
Wherein the persulfate (such as sodium persulfate solution), Fenton's reagent, permanganate and other oxidizing agents can treat most organic matters such as petroleum hydrocarbon, BTEX (benzene, toluene, ethylbenzene, xylene), phenols, MTBE (methyl tert-butyl ether), chlorinated organic solvent, polycyclic aromatic hydrocarbon, pesticides and the like, and zero-valent iron, ferrous ions, sulfide, sulfite and other reducing agents can treat heavy metals (such as hexavalent chromium), chlorinated organic matters and the like.
The temperature of the soil system can be raised by controlling the anode and the cathode of the electrode and increasing the content of electrolyte in the soil system, and persulfate can be activated. Therefore, the mass transfer advantage of the electrodynamic force in the viscous soil is utilized to drive the persulfate and other repair agents to fully contact and react with organic pollutants; meanwhile, the persulfate is activated by utilizing the heat generated by the electric process through a regulation and control means, so that the oxidation capacity and the repair efficiency of the persulfate can be obviously improved, other exogenous substances are not introduced, the operation is simple and easy to implement, and the technical significance is good. The method not only can solve the problem of poor persulfate transfer capacity in the viscous soil, but also solves the problem of difficult activity of the persulfate under the field condition, thereby not only avoiding the defect that the electric repair technology is difficult to apply, but also enhancing the in-situ mass transfer capacity of the chemical oxidation method, and simultaneously solving the problem of in-situ activation and efficiency enhancement of the persulfate in the same system.
Detailed Description
The invention is illustrated below by means of specific examples, without being restricted thereto.
The soil to be treated is high-viscosity and low-permeability soil, and the main pollutant is polycyclic aromatic hydrocarbon (mainly phenanthrene which is one of PAHs difficult to oxidize). Five areas with similar contaminant types and concentrations were selected for repair tests (including examples and comparative examples), respectively.
Example 1
The concrete repairing steps are as follows:
1) pumping the sodium persulfate solution in the chemical tank into an injection well which extends into the soil to be repaired by 1 meter through a pipeline;
2) respectively inserting a cathode and an anode (adopting an electrode system of patent CN 106881346A) connected with a power supply into soil to be treated, electrifying to form an electric field, and driving sulfate radicals to realize transmission in the soil by electric power;
3) heating and temperature rising can be realized through power supply regulation, and the specific power supply regulation and control method comprises the following steps:
injecting electrolyte into the electrode system, wherein the electrolyte is a mixed solution of sodium persulfate and sodium chloride, the concentration of the sodium persulfate and the concentration of the sodium chloride are both 1.0mol/L, and continuously updating by using an electrolyte circulating system;
switching on a power supply, and gradually adjusting the voltage gradient between the two electrodes from 0V/cm to 1.5V/cm;
monitoring the temperature change of the soil between the two electrodes, wherein the average temperature of the soil rises to 40 ℃ after 3 hours, and the reaction starts to occur;
after starting for 6 hours, switching the electrodes to gradually raise the average temperature of the soil to nearly 60 ℃, wherein the reaction is relatively fast;
thereafter, the electrodes were switched every 6 hours, maintaining the average temperature of the soil between 40-60 ℃ and running for 24 hours.
And finally, 5 point soil with equal distance between the two electrodes is collected for detection and analysis.
Example 2
The concrete repairing steps are as follows:
1) pumping the sodium persulfate solution in the chemical tank into an injection well which extends into the soil to be repaired by 1 meter through a pipeline;
2) inserting a cathode and an anode which are connected with a power supply into soil to be treated respectively, electrifying to form an electric field, and driving an oxidation/reduction agent to be transmitted in the soil by electric power;
3) the heating and temperature rising are realized through power supply regulation, and the specific power supply regulation and control method comprises the following steps:
injecting electrolyte into the electrode system, wherein the electrolyte is a mixed solution of 1.0mol/L sodium persulfate, 2.0mol/L sodium chloride and 0.25% Tween80, and continuously updating by using an electrolyte circulating system;
switching on a power supply, and gradually adjusting the voltage gradient between the two electrodes from 0V/cm to 2V/cm;
monitoring the temperature change of the soil between the two electrodes, wherein the average temperature of the soil rises to 50 ℃ after 1.5 hours, and the reaction starts to occur;
after 8 hours, the electrode is switched, the average temperature of the soil is gradually increased to 70 ℃, and the reaction is relatively fast;
thereafter, the electrodes were switched every 8 hours, maintaining the average temperature of the soil between 50-70 ℃ and the run was continued for 24 hours.
And finally, 5 point soil with equal distance between the two electrodes is collected for detection and analysis.
Comparative example 1
Only the sodium persulfate solution serving as the oxidizing agent is injected into the soil for remediation, and the electric drive and electrothermal activation technology is not adopted. After 24 hours, soil was detected by collecting 5 equally spaced spots on any line equidistant from the two electrodes of examples 1 and 2, centered on the injection spot.
Comparative example 2
The repairing steps are the same as the first step and the second step of the example 1, but electrothermal activation is not adopted, namely heating is not carried out, the operation is continuously carried out for 24 hours, and finally 5 point soil with equal distance between two electrodes is collected for detection and analysis.
And (3) detection results:
(1) in example 1, the removal rate of the five points PAH (PHE) is 50-70%;
(2) in example 2, the removal rate of the five point positions PAH (PHE) is 65-85%;
(3) the removal rate of the five points PAH (PHE) in the comparative example 1 is between 0 and 15 percent;
(4) in the comparative example 2, the removal rate of the five points PAH (PHE) is 35-60%.
The results show that the method is feasible to degrade organic pollutants in soil by using electric driving thermal activation, and compared with a direct flood irrigation method, the remediation efficiency is greatly improved.
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 (4)
1. An electric power driving and electric heating activation oxidation/reduction repairing method is characterized in that the method is used for treating organic pollutants in high-viscosity and low-permeability soil and specifically comprises the following steps:
injecting persulfate into soil to be treated;
inserting a cathode and an anode which are connected with a power supply into the soil to be treated respectively, electrifying to form an electric field, and driving persulfate to realize transmission in the soil through electric power, wherein the electric power is driven in a constant voltage mode, and the voltage gradient is set to be 0-5V/cm;
thirdly, through electric heating activation, charged ions in the system move and collide with each other to convert electric energy into heat energy, heating and warming are realized, persulfate can be activated after the temperature rises, and soil remediation is realized;
the electrothermal activation is to inject electrolyte into an electrode system, wherein the electrolyte is a mixed solution of 1.0mol/L persulfate and 1.0-2.0mol/L strong electrolyte, and the strong electrolyte is at least one selected from sodium chloride and potassium chloride;
the molar ratio between the persulfate and the strong electrolyte in the step is 1: 1-5.
2. The method as claimed in claim 1, wherein the acidity of the soil to be treated is controlled to be between 3 and 8.
3. The method of claim 1, wherein said electro-thermal activation further comprises electrode switching.
4. The method of claim 3, wherein the switching frequency of the electrode switching is once in 6-12 hours.
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| CN110918632B (en) * | 2019-09-20 | 2020-06-23 | 河北工业大学 | Method for restoring organic contaminated soil by using electrothermal activated persulfate |
| CN111112324B (en) * | 2019-12-20 | 2021-09-03 | 清华大学 | Organic pollutant treatment device and equipment in soil and underground water |
| CN111842471B (en) * | 2020-07-24 | 2022-04-05 | 中国科学院广州地球化学研究所长沙矿产资源勘查中心 | Method for restoring farmland soil heavy metal substances by combining chemical activation and electric ionization |
| JP7216748B2 (en) * | 2021-01-20 | 2023-02-01 | プライムプラネットエナジー＆ソリューションズ株式会社 | Liquid composition and method for manufacturing non-aqueous electrolyte secondary battery |
| CN114082776B (en) * | 2021-10-14 | 2022-07-01 | 生态环境部南京环境科学研究所 | Electric diffusion-electric heating activation method for repairing organic contaminated soil |
| CN114378112A (en) * | 2022-01-12 | 2022-04-22 | 江苏大地益源环境修复有限公司 | In-situ electric Fenton system and method for repairing organic matters in soil |
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