CN115430696A - Dry decontamination method for radioactive contaminated soil containing cesium-137 - Google Patents
Dry decontamination method for radioactive contaminated soil containing cesium-137 Download PDFInfo
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- CN115430696A CN115430696A CN202210974022.2A CN202210974022A CN115430696A CN 115430696 A CN115430696 A CN 115430696A CN 202210974022 A CN202210974022 A CN 202210974022A CN 115430696 A CN115430696 A CN 115430696A
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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
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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
Abstract
The invention belongs to the technical field of radioactive decontamination, and relates to a dry decontamination method for radioactive contaminated soil containing cesium-137. The dry decontamination method comprises the following steps: (1) Adding the radioactive contaminated soil containing cesium-137 into a magnetic separator, and performing dry treatment of 360-degree rotation and bidirectional oscillation; (2) Mixing the radioactive contaminated soil containing cesium-137 after dry treatment with magnetized zeolite and then carrying out adsorption treatment; (3) And (3) separating the magnetized zeolite from the soil by rotating the mixture subjected to adsorption treatment in a magnetic separator by 360 degrees and oscillating the mixture in two directions. By utilizing the dry decontamination method for the radioactive contaminated soil containing the cesium-137, the cesium-137 can be removed from the radioactive contaminated soil containing the cesium-137 more efficiently.
Description
Technical Field
The invention belongs to the technical field of radioactive decontamination, and relates to a dry decontamination method for radioactive contaminated soil containing cesium-137.
Background
With the rapid development of nuclear technology and nuclear industry, radioactive contamination of soil is caused by various reasons, such as nuclear leakage accidents (including leakage of waste liquid conveying pipelines and mistaken discharge of waste liquid) during the operation of nuclear facilities. The radioactive nuclide in the polluted soil can further migrate, diffuse and permeate into the surrounding environment along with the change of natural conditions, thereby causing long-term serious harm to the ecological environment and human health.
137 Cs, one of the most important fission product nuclides, is widely used as various radioactive sources and the like because of its long half-life, high branching ratio, and easy environmental entry of gamma rays (661.67 keV) with moderate energy. Therefore, the temperature of the molten metal is controlled, 137 cs is widely present in spent fuel post-treatment waste liquid, nuclear power operation waste liquid, nuclear facility decontamination decommissioning waste liquid and laboratory waste liquid, so that Cs is also a main radioactive pollution nuclide for polluting soil.
For example, the project of 'partial middle-placed pipeline and pipe ditch demolition' of the Chinese atomic energy science institute has excavated the polluted soil about 81.7m 3 The main contaminating nuclides are 137 Cs、 90 Sr、 60 Co and a small amount of 125 Sb、 241 Am with a maximum specific activity of 10 5 Bq/kg、10 3 Bq/kg、10 3 Bq/kg、 10 2 Bq/kg and 10 2 Bq/kg. It follows that the radioactivity in the contaminated soil is mainly due to 137 Cs is provided.
Foreign decontamination technology research on radioactive contaminated soil starts in the eighties of the last century, and various radioactive contaminated soil decontamination technologies, such as chemical decontamination, physical decontamination and other types of decontamination technologies, have been developed mainly by referring to the technical experiences of soil treatment for heavy metal ion contamination. Wherein the chemical decontamination mainly comprises chemical extraction, electrokinetic decontamination, heap leaching and the like; physical decontamination mainly comprises screening, flotation, separation Systems (SGS) based on the distribution relation of soil particle size and pollution nuclides, in-situ glass solidification and the like; the physical and chemical comprehensive treatment decontamination mainly comprises soil cleaning, thermal desorption and the like; in addition, soil bioremediation includes phytoremediation, microbial remediation and other technologies.
The soil cleaning is a decontamination technology developed aiming at the research of radioactive contaminated soil, the treatment cost is low, the process is simple, the applicability is wide, and the technology is mature, but the secondary waste amount is a key problem influencing the further development of the technology. Other soil treatment technologies, except screening and separation gating, are in the experimental research stage.
By preparing the efficient magnetized zeolite composite adsorbing material, cesium in soil is adsorbed, radioactive soil is decontaminated, and the adsorbent is recycled through magnetic separation, so that the soil decontamination efficiency can be greatly improved, secondary waste is reduced, the treatment cost of polluted soil is reduced, the degradation release and volume reduction of most of soil are realized, the storage pressure of a solid waste warehouse can be relieved, and the current environmental problem can be solved.
The High Gradient Magnetic Separation (HGMS) method is mainly used for separating magnetized components from soil, liquid and gas, and the process flow principle is shown in figure 1. Typically, the contaminated material is treated with water to form a slurry and passed through a magnetising column in which a magnetic field gradient is created using a ferromagnetic grid material such as steel wool or nickel foam, ferromagnetic or paramagnetic particles are attracted from the slurry through the ferromagnetic grid, diamagnetic components and liquid are passed through the magnetising column and the attracted particles are washed out of the grid when the magnetic field is switched off. According to the results of foreign tests, the treated soil has the advantage that more than 95% of paramagnetic contaminated nuclides can be removed from the simulated soil; this system does not work effectively when the pH of the slurry is 10, and the desired results are obtained when the pH is 8 and 4.
The HGMS has the advantages of less secondary waste, large volume reduction of waste, mixed waste treatment, high operation safety and suitability for being combined with other treatment technologies.
Magnetized zeolite in university of property of Japan for Cs in soil + In the adsorption experiment (see the principle in FIG. 2, 17 is soil particles, 19 is Cs) + 11 is a magnetized Na-P1 zeolite complex, 21 is a magnetic drum, 23 is a drum separator, and both 21 and 23 constitute a magnetic separator), 3000G was usedNeodymium magnets (small permanent magnets with such high magnetic induction are not available in the domestic market), indicating that increasing the magnetic induction of the magnetic cylinder is expected to enhance the separation effect of the magnetized zeolite and its treatment effect on contaminated soil.
Disclosure of Invention
The invention aims to provide a dry decontamination method for radioactive contaminated soil containing cesium-137, so as to be capable of removing the cesium-137 from the radioactive contaminated soil containing cesium-137 more efficiently.
To achieve this object, in a basic embodiment, the present invention provides a dry decontamination method for radioactive contaminated soil containing cesium-137, said dry decontamination method comprising the steps of:
(1) Adding the radioactive contaminated soil containing cesium-137 into a magnetic separator, and performing dry treatment of 360-degree rotation and bidirectional oscillation;
(2) Mixing the radioactive contaminated soil containing cesium-137 after dry treatment with magnetized zeolite and then carrying out adsorption treatment;
(3) And (3) separating the magnetized zeolite from the soil by rotating the mixture subjected to adsorption treatment in a magnetic separator by 360 degrees and oscillating the mixture in two directions.
The relevant principle of the invention is as follows:
uses a 360-degree rotation and bidirectional oscillation magnetic separator (magnetic barrel separation device) with higher separation effect to separate Cs + The method comprises the steps of carrying out dry treatment on the polluted soil waste, adopting novel Na-P1 type magnetized zeolite (the content of magnetite is 12-15 wt%), carrying out Cs adsorption exchange reaction by using a mixing standing method, carrying out magnetic separation by using a rotary vibration method of a magnetic separator, wherein the Na-P1 type magnetized zeolite has good adsorption separation effect on Cs, and the removal rate of Cs-137 can reach 90%, wherein the mass ratio of zeolite to soil is preferably 0.5 + The water content of the polluted soil is less than or equal to 20 percent.
The separation process comprises the following steps: the method comprises the steps of putting a mixture of magnetized zeolite and soil into a magnetic separator, rotating and vibrating the magnetic separator to realize full separation, opening a cover of the magnetic separator to dump a product phase, magnetically attracting a waste phase on a thin-wall nonmagnetic inner cylinder, and then drawing out the thin-wall nonmagnetic inner cylinder to dump the waste phase.
The magnetic separation operation is based on the premise that zeolite and soil particles can keep good fluidity in a system. The particles form a suspension system through oscillation in a liquid environment, and the distance between the particles is enlarged, and the electrostatic attraction is eliminated to a greater extent by water. Under the external magnetic field, the magnetic particles in the suspension have small resistance to gather to the magnetic surface, and the relatively sufficient and complete magnetic separation can be realized. When the water content of the particle mixture is small or the particle mixture is completely dry, the migration of the magnetic particles to the magnetic surface under the external magnetic field is hindered by the physical resistance and the electrostatic attraction of other particles, and the separation effect is poor.
The magnetic separator is designed into a cylinder, the cylinder surface is a magnetic surface, and two end surfaces are non-magnetic surfaces. When the device runs, the device rotates and vibrates in the radial direction, and the operation mode is intermittent operation. The magnetic separator is designed into a cylinder shape, so that the largest contact area between particles and a magnetic surface can be obtained under the condition of fixing the single treatment volume, the steric hindrance effect caused by the close packing of the magnetic particles on a small area is avoided, and meanwhile, the non-uniformity of momentum conduction of unloading dead angles and oscillation in a discrete phase system is also avoided. When the device works, the effect of uniform momentum transfer can be achieved only by rotating in a single direction and oscillating in a single direction; the non-magnetic surfaces at the two ends also enable the particle mixture which is vibrated and intermittently separated from the magnetic surfaces to keep better fluidity, so that the phenomenon of cover clamping in the steric effect is avoided; the entrainment of the product with respect to the magnetized zeolite can also be reduced when the product phase is discharged. The d/h design of the magnetic separator is referenced to standard beaker dimensions (h is column height and d is diameter).
The filling ratio of the zeolite and soil particle mixture in the magnetic separator has an influence on the magnetic separation effect, and a better separation effect can be obtained when the filling ratio is 10-25%. Rotation and oscillation are matched: the rotation provides a plurality of action normals for the oscillation, the loose discrete phase formed by the oscillation obtains larger flow run length in the rotation, so that the solid particle mixture with smaller water content in the magnetic separator obtains the fluidity similar to that in a suspension system, thereby improving the magnetic separation effect. Wherein, the rotation speed of the magnetic separator is 30-60rpm, when the oscillation frequency is 4 times of the rotation frequency, namely the magnetic separator rotates 90 degrees and oscillates for 1 time, so that the system forms 2-dimensional orthogonal oscillation, and a better separation effect can be achieved.
The method comprises the following specific operations: the amount of the mixture treated in one time is 10g by using a 50mL magnetic separator, the separation time is 1min by single rotation and shaking, and the whole operation time is about 15min by manual feeding and discharging. Assuming that the rotating vibration separation process and equipment of the magnetic separator are scaled up to the engineering application scale of 500L, 100kg of mixture can be processed at a time in the same proportion, and the separation is also carried out in 1 min. Because the size of the magnetic separator is increased, the linear velocity obtained when the particles in the magnetic separator rotate is increased, and the discrete phase kinetic energy obtained by vibration is unchanged, the separation effect can be expected to be better than the laboratory scale in engineering scale separation, and if mechanical feeding and discharging are used, the single-batch operation time can be less than 15min, namely the treatment capacity can be more than 400kg/hr. The process and apparatus can treat low water content magnetic mixtures, which is not currently available in other magnetic separators on the market. The impact oscillation equipment for engineering scale amplification has the defects of high noise, high equipment loss, low operation industrial safety and the like, and at the moment, mechanical oscillation is not needed, an electromagnet is used for replacing a permanent magnet for a laboratory device, and an intermittent magnetic surface is provided through intermittent high-frequency current, so that internal particles are spontaneously separated from the magnetic surface and redistributed to form a state similar to a suspension. Meanwhile, the electromagnet can provide higher magnetic induction intensity than the permanent magnet, and a good separation effect can be expected to be obtained on the weakly magnetic magnetized zeolite.
Magnetic induction of the apparatus was measured by measuring the magnetic field intensity of the inner wall of 5 magnetic separators using a millitesla WT20B type, and the results are shown in table 1.
TABLE 1 magnetic induction of the magnetic device used
| Device | Magnetic induction intensity (G) |
| 1# magnetic separator | 2331 |
| 2# magnetic separator | 2154 |
| 3# magnetic separator | 2147 |
| 4# magnetic separator | 2327 |
| 5# magnetic separator | 2178 |
As can be seen from Table 1, the magnetic induction intensity of each magnetic separator is slightly different, and the error is proved by checking to have no influence on the conclusion obtained by the research.
The magnetic induction intensity of the magnetic separator and the magnetic separation plate is similar, namely the magnetic separation plate can provide a reference value for ideal separation for the separation operation process of the magnetic separator.
The separation process is that the mixture of magnetized zeolite and soil is put into a magnetic separator, after the magnetic separator is rotated and oscillated, the cover of the magnetic separator is opened to dump the product phase, at the moment, the waste phase is magnetically attracted on the thin-wall nonmagnetic inner cylinder, and then the thin-wall nonmagnetic inner cylinder is drawn out to dump the waste phase.
In a preferred embodiment, the invention provides a dry decontamination method for radioactive contaminated soil containing cesium-137, wherein the magnetic separator is cylindrical, the cylindrical surface is a magnetic surface, and two end surfaces are non-magnetic surfaces.
In a preferred embodiment, the present invention provides a dry decontamination method for radioactive contaminated soil containing cesium-137, wherein in step (1), the rotation speed of the 360 ° rotation is 30-60rpm.
In a preferred embodiment, the invention provides a dry decontamination method for radioactive contaminated soil containing cesium-137, wherein in the step (1), the bidirectional oscillation is in the cross section direction of the magnetic separator and in the direction perpendicular to the cross section direction, and the oscillation speed is 3-5 times of the rotation speed of the rotation.
In a preferred embodiment, the present invention provides a method for dry decontamination of cesium-137 containing radioactive contaminated soil, wherein in step (1), said cesium-137 containing radioactive contaminated soil is added to a magnetic separator such that the volume thereof occupies 10 to 25% of the internal volume of the magnetic separator.
In a preferred embodiment, the present invention provides a dry decontamination method for radioactive contaminated soil containing cesium-137, wherein in step (1), the time of the dry treatment is 0.5-2min.
In a preferred embodiment, the invention provides a dry decontamination method for radioactive contaminated soil containing cesium-137, wherein in the step (2), the mass ratio of the radioactive contaminated soil containing cesium-137 to the magnetized zeolite after the dry treatment is 1.
In a preferred embodiment, the present invention provides a dry decontamination method for radioactive contaminated soil containing cesium-137, wherein in step (2), the magnetized zeolite is Na-P1 type magnetized zeolite having a magnetite content of 12 to 15wt%.
In a preferred embodiment, the invention provides a dry decontamination method for radioactive contaminated soil containing cesium-137, wherein in the step (3), the rotation speed of the rotary oscillation is 30-60rpm, and the oscillation speed is 3-5 times of the rotation speed.
In a preferred embodiment, the present invention provides a dry decontamination method for radioactive contaminated soil containing cesium-137, wherein in step (3), the time of the separation treatment is 0.5 to 2min.
The method has the beneficial effect that the cesium-137 can be more efficiently removed from the radioactive contaminated soil containing the cesium-137 by utilizing the dry decontamination method for the radioactive contaminated soil containing the cesium-137.
The invention separates soil and zeolite particles by improving a magnetic carrier methodThe process and the equipment realize the effective separation of the mixture of the zeolite and the soil, and fill up the problem that the zeolite directly treats the Cs with smaller water content + The technique of polluting soil is blank. The process does not produce liquid waste, and realizes effective volume reduction of radioactive soil waste.
The magnetic separation treatment technology of the magnetized zeolite provided by the invention has the advantages of higher cesium-137 removal rate, higher waste reduction ratio, no secondary liquid waste, low treatment cost, simple process and equipment, better technical feasibility and provides a new technology for volume reduction treatment of radioactive soil waste.
Drawings
FIG. 1 is a schematic diagram of the HGMS decontamination process flow.
Fig. 2 is a schematic diagram of an engineering application scheme of magnetized zeolite designed by university of property of Jatobe variation for treating contaminated soil.
FIG. 3 is a schematic diagram illustrating the principle of the rotation, oscillation and separation of the magnetic separator in step (3) of the present invention.
Detailed Description
The following examples are provided to further illustrate the specific embodiments of the present invention, and the principle of the magnetic separator rotating and shaking separation in the test step (3) of each example is shown in fig. 3.
Example 1: na-P1 type magnetized zeolite for Cs in soil + Adsorption experiment of
Adding amount (W) of coarse grain size magnetized zeolite (grain size of 1-3 mm) Stone (stone) ): 3.33g (XRF assay); 1wt% of Cs + Total weight of contaminated sample (W) Waste material ): 6.67g, wherein the soil sample is added in an amount W Soil for soil 5.50g, cs + Content (Cs) Starting point ) It was 0.055g.
The test steps are as follows:
(1) 1wt% of Cs + Adding the polluted sample into a magnetic separator, and performing dry processing for 1min by 360-degree rotation and bidirectional oscillation (bidirectional oscillation is the cross section direction of the magnetic separator and the direction vertical to the cross section direction);
(2) 1wt% of Cs after dry treatment + Mixing the polluted sample with the coarse-grain-size magnetized zeolite, and then performing static adsorption treatment for 24 hours;
(3) And (3) carrying out separation treatment on the magnetized zeolite and the soil for 1min in a magnetic separator through 360-degree rotation and bidirectional oscillation (the bidirectional oscillation is the cross section direction of the magnetic separator and the direction vertical to the cross section direction), and then discharging.
The treatment effect is as follows:
example 2: na-P1 type magnetized zeolite for Cs in soil + Adsorption experiment of (II)
Adding amount (W) of medium-particle-size magnetized zeolite (particle size of 60-80 meshes) Stone (stone) ): 3.33g (XRF assay); 1wt% of Cs + Total weight of contaminated sample (W) Waste material ): 6.67g, wherein the soil sample is added in an amount W Soil for soil Is 5.50g of Cs + Content (C) s start ) It was 0.055g.
The test steps are as follows:
(1) 1wt% of Cs + Adding the polluted sample into a magnetic separator, and performing dry processing for 1min by 360-degree rotation and bidirectional oscillation (bidirectional oscillation is the cross section direction of the magnetic separator and the direction vertical to the cross section direction);
(2) 1wt% of Cs after dry treatment + Mixing the polluted sample with medium-particle-size magnetized zeolite, and performing static adsorption treatment for 24h;
(3) And (3) carrying out separation treatment on the magnetized zeolite and the soil for 1min in a magnetic separator through 360-degree rotation and bidirectional oscillation (the bidirectional oscillation is the cross section direction of the magnetic separator and the direction vertical to the cross section direction), and then discharging.
The treatment effect is as follows:
example 3: dry decontamination of radioactively contaminated soil containing cesium-137
The soil polluted by radioactive cesium-137 is the soil polluted by the extremely low radioactive cesium in the institute of atomic energy science of China, and the adding amount of a soil sample (W) Soil for soil ): 10g of medium-sized magnetized zeolite with a particle size of 60-80 meshes, and the addition amount of the magnetized zeolite (W) Stone (stone) ): 3.33g. The grain diameter of the soil is 0.125-2mm, and the specific activity of Cs-137 in the radioactive soil is 6085Bq/kg.
The test steps are as follows:
(1) Adding a soil sample polluted by radioactive cesium-137 into a magnetic separator, and performing dry processing for 1min by 360-degree rotation and bidirectional oscillation (the bidirectional oscillation is the cross section direction of the magnetic separator and the direction vertical to the cross section direction);
(2) Mixing the soil sample polluted by the radioactive cesium-137 subjected to dry treatment with medium-particle-size magnetized zeolite, and then performing static adsorption treatment for 24 hours;
(3) And (3) carrying out separation treatment on the magnetized zeolite and the soil for 1min in a magnetic separator through 360-degree rotation and bidirectional oscillation (the bidirectional oscillation is the cross section direction of the magnetic separator and the direction vertical to the cross section direction), and then discharging.
The specific activity of the treated Cs-137 is 599Bq/kg, and the removal rate of the Cs-137 is 90%.
It will be apparent to those skilled in the art that various changes and modifications may be made in the present invention without departing from the spirit and scope of the invention. Thus, if such modifications and variations of the present invention fall within the scope of the claims of the present invention and their equivalents, the present invention is intended to include such modifications and variations. The foregoing examples or embodiments are merely illustrative of the present invention, which may be embodied in other specific forms or in other specific forms without departing from the spirit or essential characteristics thereof. The described embodiments are, therefore, to be considered in all respects as illustrative and not restrictive. The scope of the invention should be indicated by the appended claims, and any changes that are equivalent to the intent and scope of the claims are also intended to be included within the scope of the invention.
Claims (10)
1. A dry decontamination method for radioactive contaminated soil containing cesium-137 is characterized by comprising the following steps:
(1) Adding the radioactive contaminated soil containing cesium-137 into a magnetic separator, and performing dry treatment of 360-degree rotation and bidirectional oscillation;
(2) Mixing the radioactive contaminated soil containing cesium-137 after dry treatment with magnetized zeolite and then carrying out adsorption treatment;
(3) And (3) separating the magnetized zeolite from the soil by rotating the mixture subjected to adsorption treatment in a magnetic separator by 360 degrees and oscillating the mixture in two directions.
2. The dry decontamination method according to claim 1, characterized in that: the magnetic separator is cylindrical, the cylindrical surface is a magnetic surface, and two end surfaces are non-magnetic surfaces.
3. The dry decontamination method according to claim 1, characterized in that: in the step (1), the rotating speed of 360-degree rotation is 30-60rpm.
4. The dry decontamination method according to claim 1, characterized in that: in the step (1), the bidirectional oscillation is in the cross section direction of the magnetic separator and in the direction perpendicular to the cross section direction, and the oscillation speed is 3-5 times of the rotating speed.
5. The dry decontamination method according to claim 1, characterized in that: in the step (1), the volume of the radioactive contaminated soil containing cesium-137 is 10-25% of the internal volume of the magnetic separator after the radioactive contaminated soil is added into the magnetic separator.
6. The dry decontamination method according to claim 1, characterized in that: in the step (1), the time of the dry processing is 0.5-2min.
7. The dry decontamination method according to claim 1, characterized in that: in the step (2), the mass ratio of the radioactive contaminated soil containing cesium-137 after the dry treatment to the magnetized zeolite is 1.2-1, and the adsorption treatment time is 16-48h.
8. The dry decontamination method according to claim 1, characterized in that: in the step (2), the magnetized zeolite is Na-P1 type magnetized zeolite, and the content of magnetite is 12-15wt%.
9. The dry decontamination method according to claim 1, characterized in that: in the step (3), the rotating speed of the rotating oscillation is 30-60rpm, and the oscillation speed is 3-5 times of the rotating speed.
10. The dry decontamination method according to claim 1, characterized in that: in the step (3), the time of the separation treatment is 0.5-2min.
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| CN104379506A (en) * | 2012-04-04 | 2015-02-25 | 国立大学法人爱媛大学 | Zeolite and manufacturing method thereof, and method for selective and specific capture of cesium |
| CN109158209A (en) * | 2018-08-09 | 2019-01-08 | 中国原子能科学研究院 | The dry type permanent magnetism separation method of magnetic-particle in granulate mixture |
| CN112122000A (en) * | 2020-10-13 | 2020-12-25 | 中国地质科学院郑州矿产综合利用研究所 | Coarse-grained magnetic mineral magnetic gravity creep magnetic system construction method, magnetic system and magnetic separation equipment |
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| GB191018253A (en) * | 1910-08-02 | 1911-05-04 | Heinrich Ludwig Kessler | Improvements in Magnetic Separators. |
| US3947349A (en) * | 1975-03-14 | 1976-03-30 | Fritz Alan J | Permanent magnet high intensity separator |
| CN103002998A (en) * | 2010-07-15 | 2013-03-27 | 同和环保再生事业有限公司 | Soil cleaning method |
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