JP5767938B2 - Volume reduction method for low-level radioactive waste - Google Patents

Volume reduction method for low-level radioactive waste Download PDF

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JP5767938B2
JP5767938B2 JP2011230029A JP2011230029A JP5767938B2 JP 5767938 B2 JP5767938 B2 JP 5767938B2 JP 2011230029 A JP2011230029 A JP 2011230029A JP 2011230029 A JP2011230029 A JP 2011230029A JP 5767938 B2 JP5767938 B2 JP 5767938B2
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chloride
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JP2013088323A (en
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雅也 栗田
雅也 栗田
和彦 小谷
和彦 小谷
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新日鉄住金エンジニアリング株式会社
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The present invention relates to a volume reduction treatment method for low-level radioactive waste.

On the afternoon of March 11, 2011, a magnitude 9.0 subduction-zone earthquake (off the Pacific coast of Tohoku Earthquake) occurred off Sanriku Pacific Ocean. The massive earthquake and the subsequent large tsunami triggered damage to a number of facilities at a nuclear power plant built on the Pacific coast of Fukushima Prefecture, releasing a large amount of radioactive material into the atmosphere. As a result, a large amount of low-level radioactive waste such as rubble contaminated with radioactivity is generated.

According to the “Disaster Waste Disposal Policy in Fukushima Prefecture” published by the Ministry of the Environment, it is possible to safely incinerate even disaster waste that may have been contaminated with radioactive materials. It is said that the main ash and fly ash generated by incineration can be safely landfilled. Specifically, the main ash whose radioactive cesium concentration (total value of cesium 134 and cesium 137) is 8,000 Bq / kg or less can be landfilled at a general waste final disposal site (managed final disposal site). Incineration ash with a radioactive cesium concentration of over 8,000 Bq / kg and less than 100,000 Bq / kg is 1) landfill by installing an isolation layer, 2) landfill in a long-term durable container, 3) Landfill disposal is to be carried out at the general waste final disposal site by one of the methods of landfilling at the covered disposal site.

However, the method of incinerating low-level radioactive waste with an incinerator does not provide a sufficient volume reduction effect, and a large amount of radioactive incineration ash must be managed over a long period of time. Therefore, Patent Document 1 discloses a technology in which radioactive waste (incineration ash) after incineration is melted in a retort using microwaves, and the molten incineration ash is covered with a glass forming material to contain radioactivity. ing.
Further, in Patent Document 2, after separating non-combustible radioactive miscellaneous solid waste from flammable and flame retardant radioactive miscellaneous solid waste, pre-treatment into a size and form suitable for melting, oxidation and decomposition, respectively, Nonflammable radioactive miscellaneous solid waste is melted by plasma heating in one area, and flammable and flame-retardant radioactive miscellaneous solid waste is oxidized and decomposed on the melt overflowed in the other area, and then oxidized. A technique for producing a waste body by discharging a decomposition residue and a melt together and cooling and solidifying is disclosed.
Furthermore, in Patent Document 3, radioactive non-combustible solid waste containing organic substances is charged into a preheating furnace, and after adhering moisture and organic substances are removed by thermal decomposition under metal oxidation suppression conditions, Techniques for melting in a melting furnace are disclosed.

Japanese Patent Laid-Open No. 62-148898 Japanese Patent Laid-Open No. 9-90095 JP 2005-164320 A

According to the above conventional melting treatment method, radioactive waste is melted into a solidified body, so the volume can be reduced as compared with radioactive incinerated ash, but solidified as a radioactive substance instead of radioactive incinerated ash Because the body is generated in large quantities, a significant reduction in volume cannot be expected. In addition, in the case of the melt treatment methods described in Patent Documents 1 to 3, before the melt treatment, pretreatment such as incineration, pretreatment or preheating treatment is necessary, and it takes time to obtain a solidified body. There is also a problem.

The present invention has been made in view of such circumstances, and provides a volume reduction treatment method for low-level radioactive waste that can be further reduced in volume compared to conventional melting treatment methods and that can be easily reduced in volume. For the purpose.

In order to achieve the above object, the low-level radioactive waste volume reduction processing method according to the first aspect of the present invention gasifies low-level radioactive waste, which is waste such as radioactive rubble having a radioactive cesium concentration of 10,000 Bq / kg or less . the low-level radioactive waste by heating at less than 2000 ° C. 800 ° C. or higher, wherein the low-level radioactive waste and radioactive material adhering to the low-level radioactive waste under the original atmosphere instead was charged into the melting furnace Reacting the chlorine contained in the product to produce gasified radioactive chloride, cooling the combustible gas containing the radioactive chloride discharged from the gasification melting furnace, and the combustible A step of introducing a gas into the dust removing device A and collecting the radioactive fly ash containing the radioactive chloride by the dust removing device A.

Moreover, the volume reduction processing method of the low level radioactive waste which concerns on 2nd invention inserts the low level radioactive waste which is wastes, such as radioactive rubble whose radioactive cesium density | concentration is 10000 Bq / kg or less, into a gasification melting furnace. and by heating below the low-level radioactive waste 800 ° C. or higher 2000 ° C. under original atmosphere instead, the chlorine contained in the low-level radioactive waste the low-level radioactive waste and to have radioactive material attached to the product And generating a gasified radioactive chloride, burning a combustible gas containing the radioactive chloride discharged from the gasification melting furnace in a combustion chamber, and discharging from the combustion chamber A step of cooling the exhaust gas containing the radioactive chloride, and a step of introducing the exhaust gas into the dust removing device B and collecting the radioactive fly ash containing the radioactive chloride by the dust removing device B. It is characterized in Rukoto.

However, the radioactive cesium concentration is the total value of cesium 134 and cesium 137 , and low-level radioactive waste includes soil contaminated with radioactivity.

If only low-level radioactive waste is melted, the radioactive material remains in the molten slag, so that sufficient volume reduction cannot be achieved. Therefore, the present inventors have obtained the idea of managing fly ash having a smaller volume compared to slag, and decided to achieve significant volume reduction by transferring radioactive substances from slag to fly ash. Specifically, the radioactive substance is separated from the molten slag by reacting the radioactive substance with chlorine contained in the low-level radioactive waste and gasifying the generated radioactive chloride.

Since radioactive materials adhering to low-level radioactive waste are highly reactive, heating low-level radioactive waste containing chlorine in a reducing atmosphere to 800 ° C or higher reacts with chlorine to produce radioactive chloride. It becomes a thing. Since chloride has a low boiling point, the generated radioactive chloride is gasified and separated from the molten slag. The gasified radioactive chloride is cooled and aggregated, and is collected by the dust removing apparatuses A and B as radioactive fly ash. Since fly ash has a higher volume reduction rate than main ash, the collected radioactive fly ash is solidified into cement, making it easier to manage than in the past.
In addition, when the heating temperature in a gasification melting furnace is less than 800 degreeC, while transfer to a radioactive fly ash becomes inadequate, it is difficult for equipment to make heating temperature 2000 degreeC or more. Chlorine content uses chlorine contained in low-level radioactive waste.

Moreover, in the volume reduction processing method of the low level radioactive waste which concerns on 1st, 2nd invention, the said radioactive fly ash collected is wash | cleaned with washing water, The said washing water in which the said radioactive chloride is melt | dissolving The radioactive material may be recovered by water treatment.
Since the radioactive chloride has high water solubility, the radioactive chloride contained in the radioactive fly ash is dissolved in the washing water by washing the radioactive fly ash collected by the dust removal devices A and B with the washing water. To do. By treating this washing water with water, radioactive substances and combustible dust (char) can be separated and recovered. The recovered combustible dust can be reused as fuel.

Moreover, in the volume reduction processing method of the low level radioactive waste which concerns on 2nd invention, the said dust removal apparatus B is comprised with the 1st filtration dust collector and 2nd filtration dust collector which were arranged in series, and said 1st After collecting radioactive fly ash composed of the radioactive chloride with the filtration type dust collector, a neutralizing agent is added to the exhaust gas from which the radioactive chloride has been removed, and the non-radioactive fly ash with the second filtration type dust collector May be collected.

Further, in the volume reduction processing method for low-level radioactive waste according to the first and second inventions, the low-level radioactive waste storage area and / or the radioactive flight is prevented in order to prevent scattering of radioactive dust. It is preferable to cover the ash storage area with a building and to create a negative pressure in the building.

In the present invention, by heating low-level radioactive waste containing chlorine in a reducing atmosphere at a temperature of 800 ° C. or higher and lower than 2000 ° C., the radioactive material attached to the low-level radioactive waste is converted into gasified chloride. Transition. The gasified radioactive chloride is collected as radioactive fly ash with a high volume reduction rate. As a result, the volume can be further reduced as compared with the conventional melt treatment method, the management of radioactive material is facilitated, and the decontaminated slag can be used effectively.
Further, in the present invention, since the gasification melting furnace is used as the reduction furnace, the pretreatment in the conventional melting process is not necessary, and the volume reduction process can be easily performed.

It is a process flowchart for demonstrating the volume reduction processing method of the low level radioactive waste which concerns on the 1st Embodiment of this invention. It is a process flow figure for demonstrating the volume reduction processing method of the low level radioactive waste which concerns on the 2nd Embodiment of this invention. It is a process flowchart for demonstrating the volume reduction processing method of the low level radioactive waste which concerns on the 3rd Embodiment of this invention. It is a process flow figure for demonstrating the volume reduction processing method of the low level radioactive waste which concerns on the 4th Embodiment of this invention. It is a process flowchart for demonstrating the volume reduction processing method of the low level radioactive waste which concerns on the 5th Embodiment of this invention. It is a process flow figure for demonstrating the volume reduction processing method of the low level radioactive waste which concerns on the 6th Embodiment of this invention.

Next, embodiments of the present invention will be described with reference to the accompanying drawings for understanding of the present invention. In addition, when the element which comprises a certain embodiment has already been demonstrated in embodiment shown before that, the same code | symbol as the above-mentioned element is attached | subjected to the said element, and description of the said element is abbreviate | omitted.

[First Embodiment]
A volume reduction processing method for low-level radioactive waste according to the first embodiment of the present invention will be described with reference to FIG. The gasification melting furnace 10 used as the reduction furnace is a shaft type gasification melting furnace. By using a shaft furnace, not only can various types of low-level radioactive waste M be treated, but a reducing agent layer is formed at the bottom of the shaft furnace, so that a stronger reducing action is obtained. be able to.

In the gasification melting furnace 10, coke and limestone as a reducing agent are introduced from the upper part of the furnace together with the low-level radioactive waste M, and the slag S generated through the processes of drying, pyrolysis, combustion, and melting is discharged from the furnace bottom. Is done. The coke charged with the low-level radioactive waste M is burned at a high temperature by oxygen-enriched air blown from the tuyeres provided in the lower part of the furnace, and a high-temperature grate is formed in the lower part of the furnace. This contributes to the formation and stable melting of low-level radioactive waste M. By using oxygen-enriched air, a high temperature can be obtained, and the volatilization rate of radioactive chloride can be increased.
The input amount of coke is 1 to 30% by mass with respect to the low-level radioactive waste M, more preferably 4 to 10% by mass, and is adjusted according to the properties of the low-level radioactive waste M.
Moreover, it is preferable that the oxygen concentration of oxygen-enriched air is 28 to 40%.

The low-level radioactive waste M charged into the gasification melting furnace 10 is heated at 800 ° C. or more and less than 2000 ° C. in a reducing atmosphere containing chlorine. Thereby, radioactive substances such as radioactive cesium, radioactive iodine, and radioactive xenon adhering to the low-level radioactive waste M undergo a chemical reaction with chlorine contained in the low-level radioactive waste M to become radioactive chloride. Since the radioactive chloride has a low boiling point, it is gasified and separated from the molten slag S. Since the slag S is not radioactive (below the management level), it can be used effectively.

The gasified radioactive chloride is provided in the upper part of the gasification melting furnace 10 as combustible gas (in-furnace gas) together with combustible dust (char) and pyrolysis gas (CO, H 2 , CH 4 , CO 2, etc.). It is discharged from the pipe 11a. A spraying device 11 is installed in the middle of the pipe 11 a, and the combustible gas containing radioactive chloride discharged from the gasification melting furnace 10 is cooled to 800 ° C. or less by the spraying device 11. By cooling the combustible gas to 800 ° C. or lower, the gasified radioactive chloride is aggregated.

The combustible gas cooled by the spraying device 11 is introduced into a dust removing device A12 such as a cyclone. Aggregated radioactive chloride is collected as radioactive fly ash R together with combustible dust in the dust removing device A12, and the remaining non-radioactive combustible gas G is a combustion chamber (shown in the figure) installed at the rear stage of the dust removing device A12. Omitted).
The radioactive fly ash R collected by the dust remover A12 can be cemented and stably managed.

[Second Embodiment]
The low volume radioactive waste volume reduction processing method according to the second embodiment of the present invention will be described with reference to FIG. The second embodiment is different from the first embodiment in that a process for separating the radioactive fly ash R collected by the dust removing device A12 into the radioactive substance C and the non-radioactive combustible dust D is added.

The radioactive fly ash R collected by the dust removing device A12 is introduced into the cleaning device 16. In the cleaning device 16, the radioactive fly ash R is cleaned with the cleaning water W1. Since the radioactive chloride has high water solubility, by washing the radioactive fly ash R with the washing water W1, the radioactive chloride contained in the radioactive fly ash R is dissolved in the washing water W1, and the non-radioactive flammable dust D and To be separated. The non-radioactive combustible dust D can be used as a fuel, and when returned to the gasification melting furnace 10 and used as a fuel, the low-level radioactive waste M is not concentrated. In addition, it is preferable that the quantity of the washing water W1 with respect to the radioactive fly ash R is 10 to 50 times in mass ratio. Moreover, it is preferable that pH at the time of washing | cleaning is 5-6.

The cleaning water W1 used for cleaning the radioactive fly ash R is sent to the water treatment device 17. In the water treatment device 17, the washing water W1 in which the radioactive chloride is dissolved is treated with water and recovered as the radioactive substance C. Water treatment methods include neutralizing the wash water W1 to form a composite salt, reducing the solubility in the wash water W1 and aggregating, capturing the radioactive substance C with a chelate and aggregating and precipitating, An evaporation process or the like can be used. Alternatively, recovery using an adsorbent such as activated carbon or zeolite is also possible. In addition, it is preferable that pH after neutralization process is 6-8.
The radioactive substance C collected by the water treatment device 17 can be solidified and stably managed.
Further, the purified water W2 decontaminated by the water treatment device 17 can be reused as the cleaning water W1 in the cleaning device 16.

[Third Embodiment]
A volume reduction processing method for low-level radioactive waste according to the third embodiment of the present invention will be described with reference to FIG. In the third embodiment, unlike the first and second embodiments, the combustible gas discharged from the gasification melting furnace 10 does not pass through the spray device 11 and the dust removal device A12 and enters the combustion chamber 14. Introduced directly. Of the combustible gas introduced into the combustion chamber 14, combustible dust and pyrolysis gas are completely burned in the combustion chamber 14, and exhaust gas containing radioactive chloride is discharged from the combustion chamber 14.

The exhaust gas containing radioactive chloride discharged from the combustion chamber 14 is cooled by heat recovery in the boiler 15 and then introduced into a dust removing device B13 such as a filtration dust collector. The radioactive chloride contained in the exhaust gas is collected as radioactive fly ash R in the dust removal device B13, and the remaining non-radioactive exhaust gas E is introduced into the atmosphere from a chimney (not shown) installed at the rear stage of the dust removal device B13. Released. Steam generated by heat recovery by the boiler 15 is used as a heat source for a steam turbine generator or the like.
The radioactive fly ash R adhering to the inside of the boiler 15 is removed and collected by a striking device or a soot blower.

[Fourth Embodiment]
A volume reduction processing method for low-level radioactive waste according to the fourth embodiment of the present invention will be described with reference to FIG. In 4th Embodiment, in order to isolate | separate the radioactive fly ash R collected by the dust removal apparatus B13 in 3rd Embodiment into the radioactive substance C and the non-radioactive fly ash H, it is a washing | cleaning apparatus in the back | latter stage of the dust removal apparatus B13. 16 and a water treatment device 17 are installed.
The radioactive fly ash R introduced into the cleaning device 16 is cleaned with the cleaning water W1 in the cleaning device 16, and the non-radioactive fly ash H is recovered. On the other hand, the radioactive substance C dissolved in the washing water W <b> 1 is collected in the water treatment device 17.

[Fifth Embodiment]
A volume reduction processing method for low-level radioactive waste according to the fifth embodiment of the present invention will be described with reference to FIG. In the fifth embodiment, the dust removing device B13 in the third embodiment is configured by a first filtration type dust collector 18 and a second filtration type dust collector 19 arranged in series.

The exhaust gas containing the radioactive chloride discharged from the combustion chamber 14 is cooled by heat recovery in the boiler 15 and then introduced into the first filtration type dust collector 18. At that time, by setting the exhaust gas temperature to 80 ° C. or more and 250 ° C. or less, condensation in the filtration dust collectors 18 and 19 and burning of the filter cloth can be suppressed.
In the first filtering dust collector 18, radioactive fly ash T made of radioactive chloride is collected from the exhaust gas, and the exhaust gas from which the radioactive chloride has been removed is added with a neutralizing agent N such as slaked lime or caustic soda, It is introduced into the second filtration type dust collector 19. In the second filtration type dust collector 19, calcium chloride or the like is collected as non-radioactive fly ash H, and the remaining non-radioactive exhaust gas E is discharged from the chimney into the atmosphere. In addition, the collection rate of radioactive fly ash T can be improved by blowing activated carbon into the 1st filtration type dust collector 18. FIG.

[Sixth Embodiment]
A volume reduction processing method for low-level radioactive waste according to a sixth embodiment of the present invention will be described with reference to FIG. In the sixth embodiment, the storage area of the low-level radioactive waste M in the third embodiment is covered and airtight with the building 20, and the inside of the building 20 is made negative pressure by suction ventilation from the outside of the building 20. .

The suction-ventilated gas is supplied to the gasification melting furnace 10 or the combustion chamber 14 as combustion air. Thereby, the radioactive dust in the gas ventilated can be collected together with the radioactive fly ash R and T treated as waste. A part of the suctioned and ventilated gas can be supplied to the adsorption layer 21 made of a porous adsorbent such as activated carbon or zeolite. In the adsorption layer 21, radioactive dust is captured and the decontaminated gas is released into the atmosphere A.
The adsorbed material used can be safely managed by solidifying the cement or putting it into the gasification melting furnace 10.

Although the embodiments of the present invention have been described above, the present invention is not limited to the configurations described in the above-described embodiments, and is considered within the scope of the matters described in the claims. Other embodiments and modifications are also included. For example, in the sixth embodiment, the third embodiment is taken as an example and the technique for preventing radioactive dust from scattering has been described, but it goes without saying that the present invention can also be applied to other embodiments. Further, not only the storage area for low-level radioactive waste but also the storage area for radioactive fly ash may be covered with a building so that the building has a negative pressure.

10: Gasification melting furnace, 11a: Piping, 11: Spraying device, 12: Dust removal device A, 13: Dust removal device B, 14: Combustion chamber, 15: Boiler, 16: Cleaning device, 17: Water treatment device, 18: 1st filtration type dust collector, 19: 2nd filtration type dust collector, 20: Building, 21: Adsorption layer, A: Atmosphere, C: Radioactive material, D: Non-radioactive combustible dust, E: Non-radioactive exhaust gas, G: Non-radioactive flammable gas, H: Non-radioactive fly ash, M: Low-level radioactive waste, N: Neutralizing agent, R, T: Radioactive fly ash, S: Slag, W1: Washing water, W2: Purified water

Claims (6)

  1. Radioactive cesium concentration low level radioactive said low-level radioactive wastes less than 2000 ° C. 800 ° C. or higher waste under the original atmosphere instead was charged into the gasification melting furnace is a waste, such as less radioactive debris 10000Bq / kg By reacting a radioactive substance adhering to the low-level radioactive waste with a chlorine content contained in the low-level radioactive waste by heating at a low-level radioactive waste , and generating the gasified radioactive chloride, and the gas A step of cooling the combustible gas containing the radioactive chloride discharged from the chemical melting furnace, and introducing the combustible gas into the dust removing device A, and capturing the radioactive fly ash containing the radioactive chloride by the dust removing device A. And a process for collecting the low-level radioactive waste.
  2. Radioactive cesium concentration low level radioactive said low-level radioactive wastes less than 2000 ° C. 800 ° C. or higher waste under the original atmosphere instead was charged into the gasification melting furnace is a waste, such as less radioactive debris 10000Bq / kg By reacting a radioactive substance adhering to the low-level radioactive waste with a chlorine content contained in the low-level radioactive waste by heating at a low-level radioactive waste , and generating the gasified radioactive chloride, and the gas A step of burning a combustible gas containing the radioactive chloride discharged from the chemical melting furnace in a combustion chamber, a step of cooling the exhaust gas containing the radioactive chloride discharged from the combustion chamber, and a dust removing device for the exhaust gas And a step of collecting the radioactive fly ash containing the radioactive chloride by the dust removing device B, which is introduced into B, and a method for reducing the volume of low-level radioactive waste.
  3. 3. The volume reduction treatment method for low-level radioactive waste according to claim 1 or 2, wherein the collected radioactive fly ash is washed with washing water, and the washing water in which the radioactive chloride is dissolved is treated with water. A method for volume reduction treatment of low-level radioactive waste, characterized by collecting radioactive material by
  4. 3. The low-level radioactive waste volume reduction processing method according to claim 2, wherein the dust removing device B is constituted by a first filtration dust collector and a second filtration dust collector arranged in series, and the first filtration dust collector. After collecting the radioactive fly ash composed of the radioactive chloride in step 1, a neutralizing agent is added to the exhaust gas from which the radioactive chloride has been removed, and the non-radioactive fly ash is collected by the second filtration dust collector. A volume reduction treatment method for low-level radioactive waste.
  5. In the volume reduction processing method of the low level radioactive waste of any one of Claims 1-4, the storage area of the said low level radioactive waste is covered with a building, and the said building is made into negative pressure. A volume reduction method for low-level radioactive waste.
  6. 5. The low-level radioactive waste volume reduction processing method according to claim 1, wherein the radioactive fly ash storage area is covered with a building, and the building is under negative pressure. A volume reduction method for low-level radioactive waste.
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