CN112387772A - Method for repairing chlorohydrocarbon polluted site by in-situ chemical oxidation - Google Patents

Method for repairing chlorohydrocarbon polluted site by in-situ chemical oxidation Download PDF

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CN112387772A
CN112387772A CN202011097628.XA CN202011097628A CN112387772A CN 112387772 A CN112387772 A CN 112387772A CN 202011097628 A CN202011097628 A CN 202011097628A CN 112387772 A CN112387772 A CN 112387772A
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soil
chemical oxidation
situ chemical
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chlorinated hydrocarbon
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CN112387772B (en
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马军军
韩正昌
卜旭凌
陶志慧
朱家明
张寿兵
周啸
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Nanjing G+w Environment Engineering 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
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    • C09K17/00Soil-conditioning materials or soil-stabilising materials
    • C09K17/02Soil-conditioning materials or soil-stabilising materials containing inorganic compounds only
    • C09K17/06Calcium compounds, e.g. lime
    • BPERFORMING OPERATIONS; TRANSPORTING
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    • B09CRECLAMATION OF CONTAMINATED SOIL
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Abstract

本发明涉及一种原位化学氧化修复氯代烃污染场地的方法,先将细沙用粉喷桩机喷入地下,提高土壤砂粒的含量,改善土壤结构达到较好透水效果;再将氧化剂、催化剂和水泥的混合料用粉喷桩机喷入地下,水泥固化后将药剂包裹成团,实现其缓慢释放的目的;单独将细沙用粉喷桩机喷入地下,再将催化剂和水泥的混合料用粉喷桩机喷入地下,喷入地下水的下游位置;待水泥固化后,将过氧化氢通过注入井注入地下水的上游位置;本发明中细沙可提高土壤砂粒的含量,改善土壤结构达到较好的透水效果,固化的水泥包裹氧化剂和催化剂成团,可有效的延缓药剂的溶解,而细沙的喷入形成的透水结构,为过氧化氢与催化剂接触反应提供了良好的通道,提高氧化剂的氧化效率。

Figure 202011097628

The invention relates to a method for in-situ chemical oxidation and remediation of chlorinated hydrocarbon polluted sites. First, fine sand is sprayed into the ground with a powder pile sprayer to increase the content of soil sand particles and improve the soil structure to achieve better water permeability; The mixture of catalyst and cement is sprayed into the ground with a powder injection pile machine. After the cement is solidified, the agent is wrapped into a group to achieve the purpose of slow release; The mixture is sprayed into the ground with a powder spray pile machine and into the downstream position of the groundwater; after the cement is solidified, the hydrogen peroxide is injected into the upstream position of the groundwater through the injection well; the fine sand in the present invention can increase the content of soil sand and improve the soil The structure achieves good water permeability. The cured cement wraps the oxidant and the catalyst into a group, which can effectively delay the dissolution of the agent, and the water-permeable structure formed by the injection of fine sand provides a good channel for the contact reaction between hydrogen peroxide and the catalyst. , to improve the oxidation efficiency of the oxidant.

Figure 202011097628

Description

Method for repairing chlorohydrocarbon polluted site by in-situ chemical oxidation
Technical Field
The invention relates to a method for restoring a site polluted by chlorohydrocarbon by in-situ chemical oxidation, belonging to the field of in-situ chemical oxidation methods of soil.
Background
Chlorinated hydrocarbon solvents are used as important chemical raw materials and organic solvents and widely applied to the chemical industry. Due to the reasons of inappropriate mass production, use and storage of chlorinated hydrocarbons, chlorinated hydrocarbons enter soil and underground water and become common pollutants in the environment, particularly trichloromethane, trichloroethane, trichloroethylene, tetrachloroethylene and the like. The chlorinated hydrocarbon generally has carcinogenicity, teratogenicity and mutagenicity, and the carbon-hydrogen bond energy of the chlorinated hydrocarbon is higher, so that the chlorinated hydrocarbon can exist in the environment for a long time, and the toxic effect on the human health and the ecological environment is increased. Chlorinated hydrocarbons are mostly heavy non-aqueous phase liquids, have the characteristics of low solubility and high density, and pollute soil and underground water by taking gravity infiltration as a main power when the chlorinated hydrocarbons are leaked or discharged to the surface and underground. When the gas-coated zone soil layer enters the underground water layer and meets the 'barrier layer' with smaller permeability coefficient, the gas-coated zone soil layer is easy to stay at the top of the barrier layer and transversely diffuses along with the flow of the underground water, and further the safe utilization of the underground water in a larger range is threatened.
In-situ chemical oxidation (ISCO) is a remediation technique that introduces a chemical oxidant into an underground water environment to undergo a redox reaction with a pollutant, so that the pollutant is degraded or converted into a low-toxicity and low-mobility product, and common oxidants include permanganate, hydrogen peroxide, fenton's reagent, persulfate, ozone, and the like. However, due to the complexity of the soil structure and chemical components, humic acid, reducing metals and other substances present in the soil consume a large amount of oxidizing agents. In addition, the chemical oxidizing agent is injected into the soil in an area with non-directional migration direction and range and poor soil layer permeability, so that the transmission rate of the chemical oxidizing agent is low, and the oxidation efficiency is affected.
Based on the problems in the prior art, the invention provides a method for repairing a typical chlorinated hydrocarbon polluted site in soil by in-situ chemical oxidation.
Disclosure of Invention
The invention provides a method for repairing a chlorinated hydrocarbon polluted site by in-situ chemical oxidation aiming at the defects in the prior art, and aims to solve the problems in the prior art.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
a method for restoring a site polluted by chlorohydrocarbon by in-situ chemical oxidation comprises the following steps:
(1) firstly, spraying a fine sand powder spraying pile foundation into a specific soil depth to improve a soil mechanism and improve the water permeability of soil;
(2) uniformly mixing calcium peroxide, persulfate, ferrous sulfate and cement, spraying the mixture into the ground through a powder spraying pile machine, solidifying and wrapping the mixture into clusters by using the cement to form a coating-like effect, and prolonging the oxidation effect of an oxidant;
(3) spraying fine sand into soil of a polluted site by a dry method by using a powder spraying pile machine; then separately and uniformly mixing the ferrous sulfate catalyst and the cement, and spraying the mixture into the soil of the polluted site by a dry method through a powder spraying pile machine;
(4) after cement in the soil is solidified, hydrogen peroxide liquid oxidant is injected into the upstream area of underground water in the soil of the polluted site through an injection well and diffuses towards the downstream of underground water migration under the natural migration effect of the underground water.
(5) A plurality of injection wells are deployed in the field, and the ends of the injection wells do not penetrate the water barrier.
Furthermore, the adding amount of the fine sand in the step (1) is 50 kg-180 kg/m of each pile3
Further, the molar ratio of the addition amount of the calcium oxide to the addition amount of the ferrous sulfate in the step (2) is 10-20: 1, and the molar ratio of the addition amount of the persulfate to the addition amount of the ferrous sulfate is 2-10: 1.
Further, the molar ratio of the total addition of the calcium peroxide and the persulfate in the step (2) to the content of the chlorinated hydrocarbon in the polluted soil is 8-10: 1; the mass ratio of the calcium peroxide to the persulfate is 1: 2-4.
Further, the adding amount of the cement in the step (2) is 60-150 kg/m of each pile3
Further, the molar ratio of the adding amount of the ferrous sulfate in the step (3) to the adding amount of the hydrogen peroxide in the step (4) is 5-20: 1.
Further, the hydrogen peroxide in the step (4) is hydrogen peroxide liquid with the mass fraction of 20-30%; the molar ratio of the addition amount of the hydrogen peroxide to the content of the chlorinated hydrocarbon in the polluted soil is 5-10: 1.
Further, the adding amount of the fine sand in the step (3) is 50 kg-180 kg/m of each pile3
Further, the adding amount of the cement in the step (3) is 60-150 kg/m of each pile3
Further, the ferrous sulfate in the steps (2) and (3) has a particle size of 6-20 meshes.
The in-situ chemical oxidation repair technology adopts a mode of combining a solid chemical oxidant and a liquid chemical oxidant, uses calcium peroxide, persulfate and hydrogen peroxide as an oxidant group, and uses ferrous sulfate as a catalyst. The calcium peroxide and the persulfate are solid or powder particle reagents, the hydrogen peroxide is a liquid reagent with the concentration of 20-30%, and the ferrous sulfate is a solid particle reagent.
After being uniformly mixed with cement, the solid or powder particle oxidant and the solid particle catalyst are injected into soil in a spraying mode of a powder-spraying pile machine, and the cement achieves the effect similar to 'coating' after being solidified; the liquid reagent is injected into the underground through an injection well, and is mixed with soil and underground water to generate chemical oxidation reaction by utilizing the natural migration characteristic of the underground water.
According to the field pollution condition, a plurality of solid oxidant injection point positions can be distributed according to a grid method or a plum blossom method and the like, fine sand is injected underground in a preferential injection mode, and then the solid oxidant, the catalyst and the cement are mixed and injected underground. And (3) arranging an injection well according to the flow direction of underground water in the polluted site, and arranging a ferrous sulfate catalyst at the downstream position of the underground water of the injection well to form a finished product character.
The liquid reagent is injected underground through an injection well, the depth of the injection well does not penetrate through a water-resisting layer, and the situation that pollutants move downwards along with the injection well due to the fact that the injection well penetrates through the water-resisting layer is prevented, and the pollution depth and the pollution range are further expanded.
The liquid oxidant meets the slowly-released catalyst in the process of moving downstream under the action of groundwater dynamic force, so that a large number of hydroxyl free radicals can be released, the reaction rate of the oxidant is improved, and the reaction time of the oxidant and pollutants is prolonged. In addition, the slowly released catalyst encounters the released solid oxidant to carry out catalytic reaction again in the process of underground water migration, so that the oxidation efficiency of the solid oxidant is improved.
Compared with the prior art, the invention has the following beneficial effects because the technology is adopted:
1. according to the invention, the content of sand grains in the soil is increased through the injection of the fine sand, the soil structure is improved, and the water permeability of the soil is enhanced. The cement is solidified to form a solidified substance which can effectively wrap solid or powder chemical agents, the dissolution and release of the chemical agents are delayed, and the solidified substance can react with a hydrogen peroxide liquid oxidant injected into an injection well by matching with a good permeable structure formed by fine sand, so that the oxidation efficiency of a chemical oxidant group is further improved.
2. The catalyzed solid oxidant and the catalyzed liquid oxidant can obtain higher oxidation potential, calcium peroxide and hydrogen peroxide can release a large amount of hydroxyl free radicals to degrade chlorinated hydrocarbon pollutants, and the oxidation capacity of the hydrogen peroxide and persulfate is greatly improved under the catalytic action of ferrous sulfate.
3. The cement, the fine sand and the solid reagent injected by powder spraying are mixed with the natural soil body, the reference of the cement and the fine sand is controlled, the solidified structure can be formed but has lower strength, and the solid oxidant and the catalyst ferrous sulfate which are wrapped by the solidified cement can be slowly released after being eroded by underground water.
Drawings
Fig. 1 is a schematic view of the layout of a contaminated site.
Detailed Description
The invention is further elucidated with reference to the drawings and the detailed description.
Example 1:
a method for restoring a site polluted by chlorohydrocarbon by in-situ chemical oxidation comprises the following steps:
1. according to the situation of a polluted site, solid oxidant points and liquid oxidant injection wells are arranged at equal intervals according to a grid method.
2. The molar ratio of the total addition amount of the solid oxidant to the concentration of the chlorinated hydrocarbon site pollutants is 8:1, and the mass ratio of the calcium peroxide to the persulfate oxidant is 1: 2.
3. Before the solid oxidant is sprayed into the ground, the fine sand is firstly injected into the ground by using a powder-jet pile driver, and the injection quantity is 80kg/m per pile3
4. The dosage of the catalyst ferrous sulfate injected underground along with the solid oxidant adopts: the molar ratio of the added calcium peroxide to the added ferrous sulfate is 20:1, and the molar ratio of the added persulfate to the added ferrous sulfate is 10: 1.
5. the dosage of the underground cement injected together with the solid oxidant is 90kg/m per pile3
6. Before the ferrous sulfate catalyst is sprayed into the ground, the fine sand is injected into the ground by means of powder-spraying pile driver, and the injection quantity is 100kg/m per pile3
7. The injection amount of the separately sprayed catalyst ferrous sulfate was: the molar ratio of the amount of the ferrous sulfate catalyst to the amount of the hydrogen peroxide liquid oxidant is 5: 1.
8. The dosage of the underground cement injected together with the solid catalyst is 60kg/m per pile3
9. After cement is solidified, the total amount of the injected hydrogen peroxide liquid oxidant with the mass fraction of 28 percent is diluted into diluent with the volume fraction of 5 percent according to the mol ratio of 5:1 to the chlorinated hydrocarbon pollutant in the polluted soil, the diluent is injected into the upstream area of the underground water in the soil of the polluted site in 8 times of equal amount, the injection time interval is 7d, and the depth of an injection well does not penetrate through a water-resisting layer.
The liquid oxidant meets the slowly released catalyst in the process of moving downstream under the action of groundwater dynamic force, and the slowly released catalyst meets the released solid oxidant in the process of moving the groundwater to perform catalytic reaction again.
In this embodiment, the ferrous sulfate has a particle size of 6-20 mesh.
Example 2:
a method for restoring a site polluted by chlorohydrocarbon by in-situ chemical oxidation comprises the following steps:
1. according to the situation of a polluted site, solid oxidant points and liquid oxidant injection wells are arranged at equal intervals according to a plum blossom method.
2. The molar ratio of the total addition amount of the solid oxidant to the concentration of the chlorinated hydrocarbon site pollutant is 10:1, and the mass ratio of the calcium peroxide to the persulfate oxidant is 1: 4.
3. Before the solid oxidant is sprayed into the ground, the fine sand is firstly injected into the ground by using a powder-jet pile driver, and the injection quantity is 160kg/m per pile3
4. The dosage of the catalyst ferrous sulfate injected underground along with the solid oxidant adopts: the molar ratio of the added calcium peroxide to the added ferrous sulfate is 10:1, and the molar ratio of the added persulfate to the added ferrous sulfate is 2: 1.
5. the dosage of the underground cement injected together with the solid oxidant is 100kg/m per pile3
6. Before the ferrous sulfate catalyst is sprayed into the ground, the fine sand is injected into the ground by using a powder-spraying pile machine, and the injection amount is 120kg/m per pile3
7. The injection amount of the separately sprayed catalyst ferrous sulfate was: the molar ratio of the amount of ferrous sulfate catalyst to the amount of liquid hydrogen peroxide oxidant added is 20: 1.
8. The dosage of the underground cement injected together with the solid catalyst is 80kg/m per pile3
9. After cement is solidified, the total amount of injected hydrogen peroxide liquid oxidant with the mass fraction of 20 percent is diluted into diluent with the volume fraction of 4 percent according to the mol ratio of 10:1 to chlorinated hydrocarbon pollutant in the polluted soil, the diluent is injected into the upstream area of underground water in the soil of a polluted site in 10 times and equal amount, the injection time interval is 10d, and the depth of an injection well does not penetrate through a water-resisting layer.
The liquid oxidant meets the slowly released catalyst in the process of moving downstream under the action of groundwater dynamic force, and the slowly released catalyst meets the released solid oxidant in the process of moving the groundwater to perform catalytic reaction again.
In this embodiment, the ferrous sulfate has a particle size of 6-20 mesh.
The liquid oxidant meets the slowly released catalyst in the process of moving downstream under the action of groundwater dynamic force, and the slowly released catalyst and the solid oxidant released downstream of groundwater movement are subjected to catalytic reaction again.
TABLE 1 monitoring results of the concentration of pollutants in the soil for chemical oxidation remediation of chlorinated hydrocarbons in a chemical field
Figure BDA0002724272770000051
Note: the restoration target value is a screening value of a second-class land according to soil pollution risk management and control standard (trial) of soil environment quality construction land (GB 36600-2018).
The above-mentioned embodiments are merely preferred embodiments of the present invention, and should not be construed as limiting the present invention, and the scope of the present invention should be defined by the claims, and equivalents including technical features of the claims, i.e., equivalent modifications within the scope of the present invention.

Claims (10)

1.一种原位化学氧化修复氯代烃污染场地的方法,其特征在于,包括以下步骤:1. a method for in-situ chemical oxidation repairing chlorinated hydrocarbon polluted site, is characterized in that, comprises the following steps: (1)先将细沙用粉喷桩机干法喷入的污染场地的土壤中;(1) First, spray fine sand into the soil of the polluted site by dry spraying with a powder sprayer; (2)将过氧化钙、过硫酸盐、硫酸亚铁与水泥混合均匀,通过粉喷桩机干法喷入土壤中;(2) Mix calcium peroxide, persulfate, ferrous sulfate and cement evenly, and spray them into the soil by dry method with a powder spray pile machine; (3)将细沙用粉喷桩机干法喷入的污染场地的土壤中;再将硫酸亚铁与水泥混合均匀,通过粉喷桩机干法喷入污染场地土壤中;(3) The fine sand is sprayed into the soil of the polluted site by dry method with a powder spray pile machine; then the ferrous sulfate and cement are mixed evenly, and the powder spray pile machine is used to dry spray into the soil of the polluted site; (4)待注入土壤中的水泥固化后,将过氧化氢通过注入井注入至污染场地土壤中地下水的上游区域。(4) After the cement injected into the soil is solidified, the hydrogen peroxide is injected into the upstream area of the groundwater in the soil of the contaminated site through the injection well. 2.根据权利要求1所述的一种原位化学氧化修复氯代烃污染场地的方法,其特征在于:步骤(1)中细沙加入量为每根桩50kg~180kg/m32 . The method for in-situ chemical oxidation repairing chlorinated hydrocarbon polluted sites according to claim 1 , wherein the fine sand added in step (1) is 50kg-180kg/m 3 per pile. 3 . 3.根据权利要求1所述的一种原位化学氧化修复氯代烃污染场地的方法,其特征在于:步骤(2)中过氧化钙、硫酸亚铁的加入量的摩尔比为10~20:1,过硫酸盐与硫酸亚铁的加入量的摩尔比为2~10:1。3. A method for in-situ chemical oxidation repairing chlorinated hydrocarbon polluted site according to claim 1, characterized in that: in step (2), the molar ratio of the added amount of calcium peroxide and ferrous sulfate is 10-20 : 1, and the molar ratio of the added amount of persulfate and ferrous sulfate is 2 to 10:1. 4.根据权利要求1所述的一种原位化学氧化修复氯代烃污染场地的方法,其特征在于:步骤(2)中过氧化钙、过硫酸盐的总加入量与污染土壤中氯代烃含量的摩尔比为8~10:1。4. A method for in-situ chemical oxidation repairing chlorinated hydrocarbon polluted sites according to claim 1, characterized in that: in step (2), the total amount of calcium peroxide and persulfate added is the same as the amount of chlorinated hydrocarbons in the polluted soil. The molar ratio of the hydrocarbon content is 8 to 10:1. 5.根据权利要求1所述的一种原位化学氧化修复氯代烃污染场地的方法,其特征在于:步骤(2)水泥的投加量为每根桩60~150kg/m35 . The method for in-situ chemical oxidation repairing chlorinated hydrocarbon polluted sites according to claim 1 , wherein in step (2), the dosage of cement is 60-150 kg/m 3 per pile. 6 . 6.根据权利要求1所述的一种原位化学氧化修复氯代烃污染场地的方法,其特征在于:步骤(3)中硫酸亚铁的加入量与步骤(4)中过氧化氢加入量的摩尔比为5~20:1。6. A method for in-situ chemical oxidation repairing chlorinated hydrocarbon polluted sites according to claim 1, characterized in that: the amount of ferrous sulfate added in step (3) and the amount of hydrogen peroxide added in step (4) The molar ratio of 5 to 20:1. 7.根据权利要求1或6所述的一种原位化学氧化修复氯代烃污染场地的方法,其特征在于:步骤(4)中过氧化氢为质量分数20~30%的过氧化氢液体;过氧化氢的加入量与污染土壤中氯代烃含量的摩尔比为5~10:1。7. A method for in-situ chemical oxidation repairing chlorinated hydrocarbon polluted sites according to claim 1 or 6, characterized in that: in step (4), the hydrogen peroxide is a hydrogen peroxide liquid with a mass fraction of 20-30% ; The molar ratio of the added amount of hydrogen peroxide to the content of chlorinated hydrocarbons in the polluted soil is 5 to 10:1. 8.根据权利要求1所述的一种原位化学氧化修复氯代烃污染场地的方法,其特征在于:步骤(3)中细沙加入量为每根桩50kg~180kg/m3;水泥的投加量为每根桩60~150kg/m38. A method for in-situ chemical oxidation repairing chlorinated hydrocarbon polluted sites according to claim 1, characterized in that: in step (3), the amount of fine sand added is 50kg-180kg/m 3 for each pile; The dosage is 60~150kg/m 3 for each pile. 9.根据权利要求1所述的一种原位化学氧化修复氯代烃污染场地的方法,其特征在于:步骤(2)、(3)中硫酸亚铁为粒径为6~20目。9 . The method for in-situ chemical oxidation repairing chlorinated hydrocarbon polluted sites according to claim 1 , wherein the ferrous sulfate in steps (2) and (3) has a particle size of 6-20 mesh. 10 . 10.根据权利要求1所述的一种原位化学氧化修复氯代烃污染场地的方法,其特征在于:步骤(4)中在污染场地内布设的多个注入井,且注入井的末端不穿过隔水层。10 . The method for in-situ chemical oxidation repairing chlorinated hydrocarbon polluted sites according to claim 1 , wherein: in step (4), a plurality of injection wells are arranged in the polluted site, and the ends of the injection wells are not connected. 11 . through the water barrier.
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