CN107983764B - Method for repairing and improving quality of chromium-polluted soil - Google Patents
Method for repairing and improving quality of chromium-polluted soil Download PDFInfo
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- CN107983764B CN107983764B CN201711371982.5A CN201711371982A CN107983764B CN 107983764 B CN107983764 B CN 107983764B CN 201711371982 A CN201711371982 A CN 201711371982A CN 107983764 B CN107983764 B CN 107983764B
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09C—RECLAMATION OF CONTAMINATED SOIL
- B09C1/00—Reclamation of contaminated soil
- B09C1/08—Reclamation of contaminated soil chemically
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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Abstract
A chromium-contaminated soil repairing and reforming method comprises the steps of placing chromium-contaminated soil in a fluidized bed reaction device, carrying out fluidized gas phase solvent extraction reaction with a gasified organic solvent in a fluidized bed, separating a metal compound after the reaction from the soil in a gas phase state, recovering the gaseous metal compound through a condensing device, and recovering and utilizing the organic solvent through hydrogen reduction or acidification reaction; the gasified organic solvent is heated and gasified, and then reacts with the pretreated soil particles to generate a metal complex, and the heavy metal chromium in the soil is selectively extracted, so that the soil polluted by chromium is treated.
Description
Technical Field
The invention relates to a method for repairing and transforming polluted soil, in particular to a method for repairing and transforming chromium-polluted soil, which can realize the permanent removal of chromium in the process of repairing and upgrading cadmium-polluted soil and further improve the soil environment, and belongs to the technical field of ecological management and environmental repair.
Background
Soil is an organic component of an ecological environment system and is the most important and basic comprehensive natural resource for human survival and development. The soil not only provides mechanical support capability for plant growth, but also can provide fertility factors such as water, fertilizer, gas, heat and the like required by the growth and development of the plant. However, with the rapid development of industrialization in China, soil pollution is severe due to unreasonable mining of mineral resources and smelting discharge thereof, sewage irrigation and sludge application to soil for a long time, atmospheric sedimentation caused by artificial activities, application of chemical fertilizers and pesticides, and the like. At present, China is one of the most serious countries in the world with soil pollution. According to the data published by the ministry of environmental protection in 2006, about 1.5 hundred million acres of polluted cultivated land in China account for 8.3 percent of 18 hundred million acres of cultivated land. How to protect land in China, restore soil pollution, establish a virtuous circle ecosystem and realize harmony and unity of economic, environmental and social benefits becomes an important problem to be solved urgently at present.
Different sources of contamination require different materials and methods to handle. The existing treatment methods mainly comprise various methods such as physical repair, chemical repair, biological repair, composite repair and the like. The composite repairing method has good comprehensive effect and low possibility of secondary pollution, but has higher cost and more complex equipment. Moreover, the drugs or the proportion of the drugs to be administered are different for different soils, so that different treatment equipment is required for treatment, and the equipment cost is high.
In the treatment of heavy metal contaminated soil, there are similar inventions, for example, patent CN101712042A discloses a direct thermal desorption apparatus for separating organic substances from contaminated soil and treating the organic substances by primary heating and secondary heating, which requires special fuel for primary and secondary heating during the implementation process, and is very disadvantageous in improvement of the economy of the apparatus, and the transferred contaminants are not completely purified. The invention patent CN101947543A provides a device for treating volatile organic compound contaminated soil by using clean tail gas of a power plant, the device adopts nontoxic steam which is subjected to cleaning treatment such as desulfurization, denitration and dust removal and the like of the power plant as a gas supply source, the high-temperature and high-humidity characteristics of the device are utilized to strengthen the thermal analysis of volatile organic pollutants in the soil, but the volatile organic pollutants are emitted to the atmosphere along with flue gas after being analyzed, so that secondary pollution is caused, and the device is not an ideal treatment scheme. Patent CN102527705A discloses a soil remediation method, which is to send the soil to be remediated into a rotary kiln for heating and analysis, the roasted soil is broken by a breaker and used, and the exhaust gas is discharged to the atmosphere after demercuration, combustion and dust removal.
Through searching patent documents which do not find the same technology as the invention, the following patents which have certain relation with the invention mainly exist:
1. the patent number CN200610013190.6 is an invention patent named as 'chromium-contaminated soil remediation technology', and the patent discloses a chromium-contaminated soil remediation technology: the vegetation is endowed with capillary penetration in soil for absorbing hexavalent chromium in soil (plants such as trees, lawns and the like) and a chromium-containing sewage purification technology, hexavalent chromium in polluted soil is migrated into plants or water flowing out of a percolation pool under the action of the capillary in the soil, the mutual penetration of underground water capillaries or the precipitation effect of the hexavalent chromium in the polluted soil is naturally melted, and the hexavalent chromium in the soil is restored to a safe value through carrying out purification treatment on the water in the percolation pool repeatedly.
2. The patent number is CN201710086155.5 and is named as an invention patent of 'a heavy metal chromium contaminated soil remediation method', and the patent discloses a heavy metal chromium contaminated soil remediation method, which comprises the following steps: (1) iron chips and ethanol are uniformly sprayed in the soil; (2) adjusting the pH value; (3) gamma ray radiation treatment; (4) carrying out primary spraying treatment; (5) spraying again; (6) uniformly adding a certain mass of sawdust; (7) the invention relates to a cleaning and spraying treatment method, which comprises the steps of adding scrap iron and ethanol, adjusting ph by using tartaric acid, performing radiation treatment by using gamma rays, converting hexavalent chromium into trivalent chromium, reducing chromium pollution by using the porous property of the scrap iron, removing chromium by using a mode of spraying different substances for many times, improving the removal rate of chromium and improving the soil remediation effect.
3. The invention patent with the patent number of CN201510258215.8 and the name of 'a chromium-contaminated soil remediation process' discloses a chromium-contaminated soil remediation process, which comprises the following steps: (1) adding an oxidant into the chromium-contaminated soil, and oxidizing chromium in the chromium-contaminated soil into hexavalent chromium to obtain hexavalent chromium soil; (2) adding an eluent into the hexavalent chromium soil to carry out leaching or/and leaching to obtain slightly toxic soil containing residual hexavalent chromium and an eluent containing hexavalent chromium; the leacheate is an aqueous solution containing a desorbent, and the desorbent is soluble sulfate; (3) and adding a reducing agent into the slightly toxic soil to reduce the residual hexavalent chromium to obtain the nontoxic soil. The invention has the advantages that the process can efficiently restore chromium-polluted soil without secondary pollution, sulfate is used as a desorbent, the desorption effect is better, and the economic benefit is higher.
Although the above patents relate to the restoration and reconstruction of chromium-contaminated soil, the restoration and reconstruction methods of chromium-contaminated soil are not very effective, either the cost of restoration is very high, or the restoration effect is not satisfactory, so that the method is difficult to be popularized and applied, and further improvement is still needed.
Disclosure of Invention
The invention aims to provide a method for repairing and transforming chromium-contaminated soil, which can further improve the effect of repairing the chromium-contaminated soil, realize the permanent removal of chromium in the process of repairing and upgrading the cadmium-contaminated soil, is different from the conventional curing treatment, burying and sealing and biological treatment in essence, and has the advantages of rapidness, permanent removal, compact equipment structure and the like.
In order to achieve the purpose, the invention provides a chromium-contaminated soil remediation and transformation method, which comprises the steps of placing chromium-contaminated soil in a fluidized bed reaction device, carrying out fluidized gas phase solvent extraction reaction with a gasified organic solvent in a fluidized bed, separating a metal compound after the reaction from soil in a gas phase state, recovering the gaseous metal compound through a condensing device, and recovering and utilizing the organic solvent through hydrogen reduction or acidification reaction.
Further, the gasified organic solvent is subjected to fluidized gas phase solvent extraction reaction in the fluidized bed, and the characteristics that the organic solvent with specific functional groups can chemically react with a plurality of metal compounds in the soil under certain conditions and does not react with other substances are utilized, the gasified organic solvent is heated and gasified, and then reacts with the pretreated soil particles to generate metal complexes, so that the heavy metal chromium in the soil is selectively extracted, and the soil polluted by the chromium is treated.
Further, the selective extraction of the heavy metal chromium in the soil is carried out by firstly adopting a gasifiable organic solvent, gasifying the organic solvent in a container heated to 140-220 ℃, reacting the gasified organic solvent with soil particles to be treated in a fluidized bed maintained at 200-300 ℃ for 0.5-2 hours, and filling the reacted metal compound which is still a gas-phase substance at the high temperature of 200-300 ℃ and hydrogen into a reactor to carry out a reduction reaction to generate corresponding metal and organic solvent.
Furthermore, the soil particles after pretreatment are pretreated in a fluidized bed heated at a constant temperature, in order to enable the soil particles to be in a stable fluidized state in the fluidized bed, auxiliary gas such as nitrogen and the like needs to be filled, the organic solvent is gasified and then filled into the fluidized bed together with the nitrogen, and the specific gasified organic solvent can selectively react with a plurality of metal compounds, so that the specific gasified organic solvent can be separated from the soil particles.
Further, the organic solvent is an organic chelating solvent, and comprises acetylacetone or beta-diketone diimine.
Further, the specific process steps of the chromium-contaminated soil remediation and reconstruction are as follows:
1) in order to reduce the entrainment of the material particles along with the gas and to keep the material particles in the fluidized bed in a stable fluidized state, the chromium-contaminated soil is firstly sieved until the proper particle size is 53-150 mu m;
2) adding an organic solvent (acetylacetone or beta-diketone diimine) into a temperature-controlled heating device through a peristaltic pump (the flow is controlled to be 0.2-0.4 ml/m), and controlling the temperature to be 150-200 ℃;
3) filling 50-60g of materials meeting the granularity requirement into a temperature-controllable fluidized bed, and controlling the temperature to be 200-300 ℃;
4) when the temperature of the soil in the fluidized bed reaches the specified temperature of 200-300 ℃, firstly filling nitrogen to enable the soil in the fluidized bed to enter a fluidized state;
5) mixing the gasified organic solvent with nitrogen, and allowing the mixture to enter a fluidized bed to react with soil for 0.5-2 hours;
6) the organic solvent chromium complex generated by the reaction exists in the form of vapor at 200-300 ℃, the vapor of the metal complex is filled into a specific reduction container, and reducing gas hydrogen is filled at 250-350 ℃, so that the metal complex is reduced into metal and an organic solvent;
7) recovering the organic solvent through condensation or directly returning the organic solvent to the fluidized bed device to react with the soil to be treated;
8) residual nitrogen and hydrogen in the reaction process can be recycled to the fluidized bed device to maintain the soil to be treated in the fluidized bed in a stable fluidized state.
Further, the organic solvent in the step 2) is acetylacetone or beta-diketo diimine, and is gasified in a constant-temperature heating container heated to 150-200 ℃.
Further, the organic solvent in the step 6) adopts weak acidity, and chemically reacts with heavy metal chromium in soil particles to generate a metal complex which can be gasified at a certain temperature; the metal complex can react with hydrogen under certain conditions to be reduced into recyclable organic solvent and metal.
Further, the regenerated organic solvent can be recycled.
The invention has the advantages that:
the invention has the following advantages and positive effects:
1. the process can treat chromium in the chromium-contaminated soil, fundamentally remove the chromium in the soil and radically treat the chromium contamination in the soil, is different from the traditional treatment modes such as solidification, landfill and the like, and the treated soil has no possibility of relapse.
2. The invention has the remarkable characteristic that the heavy metal chromium can be gradually enriched and even recovered through the soil treated by the process. The metal complex can be reduced with hydrogen to recover the organic solvent and the metal.
3. Has strong adaptability to various soils to be treated, and has good market prospect and popularization and application value. Can be applied to the treatment of various heavy metals in soil such as lead, nickel, cadmium and chromium.
4. In the process flow of the invention, various chemical reactions are carried out in a gas/solid phase, the organic solvent can be recycled through a gas phase reduction reaction, the whole process does not involve water, the possibility of water pollution does not exist, the gas-solid reaction must be carried out in a closed container, no harmful waste is generated in the whole process, and the process is a new green, environment-friendly and pollution-free process.
Drawings
FIG. 1 is a schematic process flow diagram of the present invention.
Detailed Description
The invention is further illustrated with reference to the following figures and specific examples.
Example one
As can be seen from the attached figure 1, the invention relates to a method for removing chromium pollution from chromium-polluted soil, which comprises the following steps:
1. sieving the soil to be treated, loading 60g of soil to be treated with proper granularity (+ 53-150 mu m) into a fluidized bed, opening a heating device, and controlling the temperature to be 240 ℃;
2. adding an organic solvent acetylacetone (0.2 ml/m) into a temperature-controlled heating device through a peristaltic pump for gasification, and controlling the temperature to be 160 ℃;
3. heating 60ml/m of nitrogen through a preheating device, filling the nitrogen into a fluidized bed device, and ensuring that particles in the fluidized bed are in a stable fluidized state after the nitrogen reaches a preset temperature;
4. loading the gasified acetylacetone into a fluidized bed, carrying out solid-gas reaction for 1.5h at the temperature of 240 ℃, carrying out chemical reaction on the acetylacetone and chromium in soil to generate an acetylacetone chromium complex, and immediately gasifying the complex at the temperature of 240 ℃;
5. the gasified acetylacetone chromium complex and hydrogen are subjected to reduction reaction in a reduction container at the temperature of 260 ℃ to generate metallic chromium and regenerated acetylacetone, the acetylacetone can be recycled and returned to the previous flow, the recovery rate/removal rate of chromium in the whole process is 78.5%, and the content of metallic chromium reaches 99.6%.
Example two
The second embodiment is basically the same as the first embodiment, except that the components and parameters are somewhat different. The method for removing chromium in soil by adopting an organic solvent beta-diketone diimine comprises the following steps:
1. screening soil to be treated, filling 70g of soil particles to be treated with proper granularity (+ 53-150 mu m) into a fluidized bed, opening a heating device, and controlling the temperature to be 240 ℃;
2. adding an organic solvent beta-diketodiimine (0.2 ml/m) into a temperature-controlled heating device through a peristaltic pump for gasification, controlling the temperature to be 180 ℃, wherein the beta-diketodiimine is adopted instead of acetylacetone in the invention, and the beta-diketodiimine has better selectivity and does not react with iron in soil mainly because of comparison with acetylacetone;
3. heating 50ml/m of nitrogen by a preheating device, filling the nitrogen into a fluidized bed device, and ensuring the particles in the fluidized bed to be in a stable fluidized state after reaching a preset temperature;
4. loading the gasified beta-diketone diimine into a fluidized bed, carrying out solid-gas reaction for 2.0h at the temperature of 240 ℃, carrying out chemical reaction on the beta-diketone diimine and chromium in soil to generate a chromium complex, and immediately gasifying the nickel complex at the temperature of 240 ℃;
5. the gasified chromium metal complex and hydrogen are subjected to reduction reaction in a reduction container at the temperature of 240 ℃ to generate metal chromium and regenerated beta-diketone diimine, the beta-diketone diimine can be recycled and returned to the previous process, the chromium removal rate in the whole process is 80.8%, and the content of the metal chromium reaches 98.7%.
It is to be clearly understood that this description is made only by way of illustration and not as a limitation on the scope of the invention, as modifications of various equivalent forms of the invention which may occur to those skilled in the art upon reading the present application are intended to fall within the scope of the appended claims.
The invention has the advantages that:
the invention has the following advantages and positive effects:
1. the process can treat chromium in the chromium-contaminated soil, fundamentally remove the chromium in the soil and radically treat the chromium contamination in the soil, is different from the traditional treatment modes such as solidification, landfill and the like, and the treated soil has no possibility of relapse.
2. The invention has the remarkable characteristic that the heavy metal chromium can be gradually enriched and even recovered through the soil treated by the process. The metal complex can be reduced with hydrogen to recover the organic solvent and the metal.
3. Has strong adaptability to various soils to be treated, and has good market prospect and popularization and application value. Can be applied to the treatment of various heavy metals in soil such as lead, nickel, cadmium and chromium.
4. In the process flow of the invention, various chemical reactions are carried out in a gas/solid phase, the organic solvent can be recycled through a gas phase reduction reaction, the whole process does not involve water, the possibility of water pollution does not exist, the gas-solid reaction must be carried out in a closed container, no harmful waste is generated in the whole process, and the process is a new green, environment-friendly and pollution-free process.
Claims (4)
1. A chromium-contaminated soil repairing and reforming method comprises the steps of placing chromium-contaminated soil in a fluidized bed reaction device, carrying out fluidized gas phase solvent extraction reaction with a gasified organic solvent in a fluidized bed, separating a metal compound after the reaction from the soil in a gas phase state, recovering the gaseous metal compound through a condensing device, and recovering and utilizing the organic solvent through hydrogen reduction or acidification reaction; the gasified organic solvent is heated and gasified, and then reacts with the pretreated soil particles to generate a metal complex, and the heavy metal chromium in the soil is selectively extracted, so that the soil polluted by chromium is treated; the method for selectively extracting the heavy metal chromium from the soil comprises the steps of firstly adopting a gasifiable organic solvent, gasifying the organic solvent in a container heated to 140-220 ℃, reacting the gasified organic solvent with soil particles to be treated in a fluidized bed at the constant temperature of 200-300 ℃ for 0.5-2 hours, enabling a reacted metal compound to be still a gas-phase substance at the high temperature of 200-300 ℃, and filling the reacted metal compound and hydrogen into a reactor to perform a reduction reaction to generate corresponding metal and organic solvent; the pretreated soil particles are pretreated in a constant-temperature heating fluidized bed, auxiliary nitrogen is required to be filled in order to enable the soil particles to be in a stable fluidized state in the fluidized bed, the fluidized bed is filled with the gasified organic solvent together with the nitrogen, and the specific gasified organic solvent can selectively react with a plurality of metal compounds so as to be separated from the soil particles; the specific process steps of the chromium-contaminated soil remediation and transformation are as follows:
1) in order to reduce the entrainment of the material particles along with the gas and to maintain the material particles in the fluidized bed in a stable fluidized state, the chromium-contaminated soil is firstly sieved until the proper particle size is 53-150 μm;
2) adding an organic solvent acetylacetone or beta-diketone diimine into a temperature-controlled heating device through a peristaltic pump, wherein the flow rate is controlled to be 0.2-0.4ml/m, and the temperature is controlled to be 150-200 ℃;
3) 50-60g of materials meeting the granularity requirement are filled into a temperature-controllable fluidized bed, and the temperature is controlled to be 200-300 ℃;
4) when the temperature of the soil in the fluidized bed reaches the specified temperature of 200-300 ℃, firstly filling nitrogen to enable the soil in the fluidized bed to enter a fluidized state;
5) mixing the gasified organic solvent with nitrogen, and reacting the mixture in a fluidized bed for 0.5 to 2 hours with soil;
6) the organic solvent chromium complex generated by the reaction exists in the form of vapor at 200-300 ℃, the vapor of the metal complex is filled into a specific reduction container, and reducing gas hydrogen is filled at 250-350 ℃, so that the metal complex is reduced into metal and an organic solvent;
7) recovering the organic solvent through condensation or directly returning the organic solvent to the fluidized bed device to react with the soil to be treated;
8) residual nitrogen and hydrogen in the reaction process are recycled to the fluidized bed device and are used for maintaining the soil to be treated in the fluidized bed in a stable fluidized state.
2. The chromium-contaminated soil remediation and reconstruction method according to claim 1, characterized in that: the organic solvent is an organic chelating solvent and comprises acetylacetone or beta-diketone diimine.
3. The chromium-contaminated soil remediation and remediation method of claim 1, wherein: the organic solvent in the step 2) is acetylacetone or beta-diketo diimine, and is gasified in a constant-temperature heating container heated to 150-200 ℃.
4. The chromium-contaminated soil remediation and remediation method of claim 1, wherein: the organic solvent in the step 6) adopts weak acidity, and chemically reacts with heavy metal chromium in soil particles to generate a metal complex which is gasified at a certain temperature; the metal complex reacts with hydrogen under certain conditions and is reduced into recyclable organic solvent and metal.
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