CN110444310B - Method for treating radioactive iodine waste - Google Patents
Method for treating radioactive iodine waste Download PDFInfo
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- CN110444310B CN110444310B CN201910643121.0A CN201910643121A CN110444310B CN 110444310 B CN110444310 B CN 110444310B CN 201910643121 A CN201910643121 A CN 201910643121A CN 110444310 B CN110444310 B CN 110444310B
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/02—Treating gases
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Abstract
The invention belongs to the technical field of radioactive waste treatment, and relates to a method for treating radioactive iodine waste. The treatment method sequentially comprises the following steps: (1) reacting the radioactive iodine waste with sodium hydroxide to obtain radioactive iodine waste conversion substance powder; (2) mixing the 4A zeolite and radioactive iodine waste conversion substance powder, grinding, drying, weighing, adding deionized water, further grinding, refining and homogenizing to obtain a uniformly wet mixture; (3) and hydrolyzing the uniformly wetted mixture, evaporating to dryness, and then heating and sintering to obtain the iodine sodalite solidified body. The method for treating the radioactive iodine waste can be used for treating the radioactive iodine waste, and has the advantages of simple process, energy conservation, environmental protection, safety and reliability.
Description
Technical Field
The invention belongs to the technical field of radioactive waste treatment, and relates to a method for treating radioactive iodine waste.
Background
The rapid development of nuclear energy is accompanied by the production of large quantities of nuclear waste, of which radioactive iodine-129/131, etc. is usually given as I-、IO3 -、I2、IO-Or CH3The I and other forms are volatilized, which causes pollution to the environment and influences the health of people.
In the early development of the nuclear industry, radioactive iodine was immobilized by adsorption, for example, in the case of the Zean of the university of Compound denier, radioactive waste gas containing radioactive iodine-129/131 was adsorbed by silver-coated silica gel. Although this method is for I2And CH3The removal efficiency of I reaches more than 99.99 percent, but the obtained silver-coated silica gel particles containing iodine are easily influenced by the environmental temperature and pH value, thereby influencing the materialStability, and the requirement of long-term disposal can not be met.
At present, the radioactive iodine treatment method mainly comprises a marine treatment method, a cement, plastic, asphalt curing method and the like. These methods can treat radioactive iodine to some extent, but have problems such as poor stability of the solidified body and secondary pollution, and thus cannot satisfy the demand for long-term treatment of radioactive iodine.
Disclosure of Invention
The invention aims to provide a method for treating radioactive iodine waste, which can treat the radioactive iodine waste in a simple process, energy conservation, environmental protection, safety and reliability manner.
To achieve this object, in a basic embodiment, the present invention provides a method for treating radioactive iodine waste, the method comprising the steps of, in order:
(1) reacting the radioactive iodine waste with sodium hydroxide to obtain a radioactive iodine waste conversion powder (3I)2+6NaOH＝5NaI+NaIO3+3H2O)；
(2) Zeolite 4A (chemical formula is Na)12[Al12Si12O48]·27H2O) mixing the powder with radioactive iodine waste conversion substance, grinding, drying, weighing, adding deionized water, further grinding, refining and homogenizing to obtain a wet and uniform mixture;
(3) and hydrolyzing the uniformly wetted mixture, evaporating to dryness, and then heating and sintering to obtain the iodine sodalite solidified body.
In a preferred embodiment, the present invention provides a method for treating radioactive iodine waste, wherein in the step (1), the mass ratio of radioactive iodine waste to sodium hydroxide is 70 to 80: 20-30.
In a preferred embodiment, the present invention provides a method for treatment of radioactive iodine waste, wherein in the step (2), the mass ratio of the 4A zeolite to the radioactive iodine waste conversion product powder is 45 to 65: 35-55.
In a preferred embodiment, the present invention provides a method for treating radioactive iodine waste, wherein in the step (2), the mass ratio of the mixture of the 4A zeolite, the radioactive iodine waste conversion product powder and the deionized water is 1:10 to 1: 5.
In a preferred embodiment, the present invention provides a method for treating radioactive iodine waste, wherein in the step (2), the average particle diameter of the solidified substance in the wet homogeneous mixture is 1 to 5 μm.
In a preferred embodiment, the invention provides a method for treating radioactive iodine waste, wherein in the step (3), the temperature for hydrolysis and evaporation to dryness is 200-250 ℃ and the time is 10-60 min.
In a preferred embodiment, the present invention provides a method for treating radioactive iodine waste, wherein in the step (3), the procedure of temperature-rising sintering is as follows: firstly heating to 400-.
In a preferred embodiment, the present invention provides a method for treating radioactive iodine waste, wherein in the step (3), the procedure of temperature-rising sintering is as follows: firstly heating to 400-450 ℃ and preserving heat for 10-15h, and then heating to 750-950 ℃ and preserving heat for 10-40 min.
The method for treating the radioactive iodine waste has the advantages that the method for treating the radioactive iodine waste is simple in process, energy-saving, environment-friendly, safe and reliable.
Detailed Description
Example 1: treatment of radioactive iodine waste
The radioactive iodine waste is treated by the following method steps:
(1) 280g of radioactive iodine waste (the source being gaseous I emitted from nuclear waste)2) Reacted with 80g of sodium hydroxide to obtain a radioactive iodine waste conversion powder.
(2) 45g of 4A zeolite and 55g of radioactive iodine waste conversion powder are mixed and ground in a colloid mill (JF-130 type Guantong mechanical Co., Ltd., Gallery), dried at 80 ℃ for 12 hours and weighed, and deionized water (solid-liquid mass ratio is 1:10) is added for further grinding, refining and homogenizing treatment to obtain a wet and uniform mixture (the average particle size of a cured substance is 1 mu m).
(3) Hydrolyzing the wet and uniform mixture in a muffle furnace (Tester instruments Co., Ltd., Tianjin, MFLC-7/12P type) to dryness (the temperature is 200 ℃, the time is 60min), heating and sintering, and naturally cooling to room temperature to obtain the iodine sodalite solidified body. The procedure of temperature-rising sintering is as follows: firstly heating to 400 ℃ and preserving heat for 15h, and then heating to 950 ℃ and preserving heat for 10 min.
XRD tests show that the prepared iodine sodalite solidified substance phase excludes main diffraction peak Na4Al3Si3O12In addition to I, a small amount of NaAlSi is also present2O6The bulk density is 2.298g/cm3The extraction rate of radionuclide I under PCT standards (the extraction rate indicates the degree of extraction of the element to be extracted, i.e., the percentage of the element extracted; see Sakuragi T, Nishimura T, Nasu Y, et al. immobilization of radioactive iodine using agricultural I vision technique for the TRU waters disporsal: evaluation of learning and surface properties [ J]MRS one Proceedings Library Archive,2008,1107.) was less than 4.23X 10 after 42 days-4g·m-2·d-1。
Example 2: treatment of radioactive iodine waste
The radioactive iodine waste is treated by the following method steps:
(1) 280g of radioactive iodine waste (the source being gaseous I emitted from nuclear waste)2) Reacted with 120g of sodium hydroxide to obtain a radioactive iodine waste conversion powder.
(2) 65g of 4A zeolite and 35g of radioactive iodine waste conversion powder are mixed and ground in a colloid mill (JF-130 type Guantong mechanical Co., Ltd., Gallery), dried at 80 ℃ for 12 hours and weighed, and deionized water (solid-liquid mass ratio is 1:5) is added for further grinding, refining and homogenizing treatment to obtain a wet and uniform mixture (the average particle size of a cured substance is 5 μm).
(3) Hydrolyzing the wet and uniform mixture in a muffle furnace (Tester instruments Co., Ltd., Tianjin, MFLC-7/12P type) to dryness (the temperature is 250 ℃ and the time is 10min), heating and sintering, and naturally cooling to room temperature to obtain the iodine sodalite solidified body. The procedure of temperature-rising sintering is as follows: the temperature is firstly increased to 450 ℃ and kept for 10h, and then the temperature is increased to 750 ℃ and kept for 40 min.
XRD tests show that the prepared iodine sodalite solidified substance phase excludes main diffraction peak Na4Al3Si3O12In addition to I, a small amount of NaAlSi is also present2O6The bulk density is 1.968g/cm3The leaching rate of the radionuclide I under the PCT standard is lower than 5.56 multiplied by 10 days after 42 days-2g·m-2·d-1。
Example 3: treatment of radioiodine waste
The radioactive iodine waste is treated by the following method steps:
(1) 320g of radioiodinated waste (the source being gaseous I emitted from nuclear waste)2) Reacted with 80g of sodium hydroxide to obtain a radioactive iodine waste conversion powder.
(2) Mixing 50g of 4A zeolite and 50g of radioactive iodine waste conversion powder, grinding in a colloid mill (JF-130 type Guantong mechanical Co., Ltd., Gallery), drying at 80 ℃ for 12h, weighing, adding deionized water (solid-liquid mass ratio is 1:8), further grinding, refining and homogenizing to obtain a wet and uniform mixture (the average particle size of a cured substance is 3 μm).
(3) Hydrolyzing the wet and uniform mixture in a muffle furnace (Tester instruments Co., Ltd., Tianjin, MFLC-7/12P type) to dryness (the temperature is 220 ℃ and the time is 30min), heating and sintering, and naturally cooling to room temperature to obtain the iodine sodalite solidified body. The procedure of temperature-rising sintering is as follows: the temperature is firstly increased to 420 ℃ and kept for 13h, and then increased to 850 ℃ and kept for 25 min.
XRD tests show that the prepared iodine sodalite has single crystalline phase and the bulk density of 2.354g/cm3The leaching rate of the radionuclide I under the PCT standard is lower than 1.78 multiplied by 10 days after 42 days-4g·m-2·d-1。
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 should be construed to be included therein.
Claims (5)
1. A method for treating radioactive iodine waste, comprising the following steps in sequence:
(1) reacting the radioactive iodine waste with sodium hydroxide to obtain radioactive iodine waste conversion substance powder;
(2) mixing the 4A zeolite and radioactive iodine waste conversion substance powder, grinding, drying, weighing, adding deionized water, further grinding, refining and homogenizing to obtain a uniformly wet mixture;
(3) hydrolyzing and evaporating the uniformly wet mixture to dryness, then heating and sintering to obtain an iodine sodalite solidified body,
wherein:
in the step (3), the temperature for hydrolysis and evaporation to dryness is 200-250 ℃, the time is 10-60min,
in the step (3), the procedure of temperature-rising sintering is as follows: firstly heating to 400-450 ℃ and preserving heat for 10-15h, and then heating to 750-950 ℃ and preserving heat for 10-40 min.
2. The processing method according to claim 1, characterized in that: in the step (1), the mass ratio of radioactive iodine waste to sodium hydroxide is 70-80: 20-30.
3. The processing method according to claim 1, characterized in that: in the step (2), the mass ratio of the 4A zeolite to the radioactive iodine waste conversion substance powder is 45-65: 35-55.
4. The processing method according to claim 1, characterized in that: in the step (2), the mass ratio of the mixture of the 4A zeolite and the radioactive iodine waste conversion substance powder to the deionized water is 1:10-1: 5.
5. The processing method according to claim 1, characterized in that: in the step (2), the average particle diameter of the solidified material in the uniformly wetted mixture is 1 to 5 μm.
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| CN111161901B (en) * | 2020-01-03 | 2022-04-05 | 中国原子能科学研究院 | Method for treating radioactive iodine waste |
| CN111584113B (en) * | 2020-04-07 | 2022-04-29 | 西南科技大学 | Solidification treatment method of radioactive zeolite waste |
| CN111986828B (en) * | 2020-08-20 | 2022-12-13 | 中国原子能科学研究院 | Sodalite-based ceramic-glass dual curing method for radioactive iodine waste |
| CN111863304B (en) * | 2020-08-20 | 2022-12-13 | 中国原子能科学研究院 | Sodalite-based ceramic curing method for radioactive iodine waste |
| CN111863305A (en) * | 2020-08-20 | 2020-10-30 | 中国原子能科学研究院 | Method for curing radioactive iodine-containing silver-coated silica gel |
| CN112201382A (en) * | 2020-10-26 | 2021-01-08 | 西南科技大学 | Low-temperature curing treatment method for radioactive silica gel waste |
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