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WO2013018512A1 - Agent pour le durcissement et la solidification du sol de surface contaminé radioactif, agent bloquant les rayonnements et procédé pour la prévention de la dispersion de substance radioactive à partir d'une surface, la décontamination et la protection - Google Patents

Agent pour le durcissement et la solidification du sol de surface contaminé radioactif, agent bloquant les rayonnements et procédé pour la prévention de la dispersion de substance radioactive à partir d'une surface, la décontamination et la protection Download PDF

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Publication number
WO2013018512A1
WO2013018512A1 PCT/JP2012/067554 JP2012067554W WO2013018512A1 WO 2013018512 A1 WO2013018512 A1 WO 2013018512A1 JP 2012067554 W JP2012067554 W JP 2012067554W WO 2013018512 A1 WO2013018512 A1 WO 2013018512A1
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curing
chemical formula
group
agent
paper
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Japanese (ja)
Inventor
岩宮　陽子
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CHOETSU KAKEN Co Ltd
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CHOETSU KAKEN Co Ltd
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    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K17/00—Soil-conditioning materials or soil-stabilising materials
    • C09K17/40—Soil-conditioning materials or soil-stabilising materials containing mixtures of inorganic and organic compounds
    • 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
    • G21F9/04—Treating liquids
    • G21F9/06—Processing
    • G21F9/16—Processing by fixation in stable solid media
    • G21F9/162—Processing by fixation in stable solid media in an inorganic matrix, e.g. clays, zeolites
    • 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
    • G21F9/28—Treating solids
    • G21F9/30—Processing
    • G21F9/301—Processing by fixation in stable solid media
    • G21F9/302—Processing by fixation in stable solid media in an inorganic matrix

Definitions

  • the present invention provides a curing / solidifying / radiation shielding agent for fixing a soil surface on which radioactive pollutants are scattered and preventing the radioactive pollutants from being scattered and capturing and removing the radioactive pollutants and It relates to decontamination and protection methods to be used.
  • radioactive pollutants Due to nuclear power reactor accidents, radioactive pollutants are scattered and humans cannot live. In such a case, in order to prevent further scattering of the scattered radioactive pollutants, for example, a synthetic resin emulsion solution made of a flying sand inhibitor cricoat made by Kurita Kogyo Co., Ltd. is sprayed and contaminated with radioactive pollutants. The surface is fixed and placed on the spot.
  • a synthetic resin emulsion solution made of a flying sand inhibitor cricoat made by Kurita Kogyo Co., Ltd. is sprayed and contaminated with radioactive pollutants. The surface is fixed and placed on the spot.
  • radioactive pollutants when radioactive pollutants are scattered on the surrounding soil surface, when the radioactive pollutants are volatile substances, for example, as disclosed in JP-A-2004-243195, “soil A pipe is embedded in the pipe, high-temperature superheated steam is jetted from the pipe into the soil, the pollutants in the soil are volatilized, and the volatiles are recovered and removed. '' Document resolution).
  • the pollutant is not a volatile substance, the contaminated surface soil is scraped off manually by human naval tactics or using heavy equipment such as a shovel car, and then removed from one place outside. It is known that decontamination of radioactive pollutants is performed by collecting in a place and removing the surface soil of the contaminated part.
  • the present invention stops the radioactive pollutants that are easily scattered, and also hardens and solidifies the radioactively contaminated soil that can very easily remove the soil surface even when removed. -To provide radiation shielding agents and prevent radioactive substances from scattering and to provide decontamination / protection methods.
  • the invention according to claim 1 of the present application is a silane-based curing / solidifying agent for curing / solidifying a radioactively contaminated soil surface, the main component compound represented by Chemical Formula 1 and a catalyst for curing / solidifying the same Hardening and solidifying agent for radioactively contaminated soil surface.
  • R 1 , R 2 , R 3 and R 4 may be the same or different, each being hydrogen or an alkyl group having 1 to 4 carbon atoms, and n is 2 to 10.
  • the invention according to claim 2 of the present application is characterized in that, in the curing / solidifying agent of claim 1, the catalyst is a hydrolyzable organometallic compound.
  • the invention according to claim 3 of the present application is the curing / solidifying agent according to claim 2, wherein the hydrolyzable organometallic compound is one or more organic compounds selected from the group consisting of titanium, zirconium, aluminum, and tin. It is a metal compound.
  • the invention according to claim 4 of the present application is the curing / solidifying agent according to any one of claims 1 to 3, further comprising three hydrolyzable substituents and one non-hydrolyzable substituent.
  • R 5 , R 6 and R 7 may be the same or different, and are hydrogen, an alkyl group or an alkenyl group, and the bond between R 5 O, R 60 and R 7 O and Si is It consists of a siloxane bond, and R 8 is an alkenyl group or a phenyl group which may contain an epoxy group or a glycidyl group (an epoxy group, a glycidyl group or an amino group) as a substituent.
  • the invention according to claim 5 of the present application is the curing / solidifying agent according to any one of claims 1 to 4, further comprising two hydrolyzable substituents and two hydrolyzable substituents.
  • R 9 and R 11 may be the same or different, and are hydrogen, an alkyl group or an alkenyl group, and the bond between R 9 O and R 11 O and Si is a siloxane bond; 10 and R 12 are an alkyl group, an alkenyl group or a phenyl group which may contain an epoxy group or a glycidyl group as a substituent.
  • the invention according to claim 6 of the present application is the curing / solidifying agent according to any one of claims 1 to 5, further comprising isopropyl alcohol (IPA), an acrylic (methacrylic) ester copolymer, and a sub-oxidation Curing / solidifying agent containing lead or lead monoxide.
  • IPA isopropyl alcohol
  • acrylic (methacrylic) ester copolymer an acrylic (methacrylic) ester copolymer
  • a sub-oxidation Curing / solidifying agent containing lead or lead monoxide (7)
  • the invention according to claim 7 of the present application is directed to the prevention and decontamination of radioactive materials on the radioactively contaminated soil surface by spraying the curing / solidifying agent of claims 1 to 6 onto the radioactively contaminated soil surface.
  • Method. is a radiation protection material obtained by immersing and drying the curing / solidifying agent according to claims 1 to 6 in Japanese paper or a fiber material.
  • the invention according to claim 9 of the present application is a radiation protection method using the radiation protection material of claim 8.
  • the invention according to claim 10 of the present application is a mixture of the curing / solidifying agent of claims 1 to 6, isopropyl alcohol (IPA), an acrylic (methacrylic) ester copolymer, and tungsten or molybdenum.
  • the invention according to claim 11 of the present application is a radiation shielding material obtained by applying or impregnating the radiation shielding agent of claim 10 to the surface of a paper material, a fiber material or a solid material.
  • the invention according to claim 12 of the present application is a mixture of the curing / solidifying agent, isopropyl alcohol (IPA), acrylic (methacrylic acid) ester copolymer, and finely powdered tungsten according to claims 1 to 6.
  • Neutron beam shielding agent is a neutron beam shielding material obtained by applying or impregnating the surface of a paper material, a fiber material, or a solid material with the neutron beam shielding agent of claim 12.
  • a radioactively contaminated soil surface can be easily sprayed and can be used as a hardening / solidifying agent for hardening / solidifying the soil surface.
  • the section is clearly radioactively decontaminated because the radioactivity intensity clearly decreases.
  • R4 in the chemical compound 1 contained in the curing / solidifying agent is not hydrolyzed even if the chemical compound 1 undergoes a subsequent hydrolysis / polycondensation reaction. It imparts water properties and, as a result, imparts water repellency to the solidified soil surface, and prevents radioactive substances in the soil from re-spraying around by water, wind, etc.
  • radioactive substances can be captured and stopped in the solidified and removed soil, and radioactive decontamination can be easily performed by moving to other places while captured. That is, since the radioactivity is measured also from the curing / solidifying agent itself, there is an effect of capturing and taking in the radioactive substance also in the medicine itself to be used.
  • the above-mentioned curing / solidifying agent itself has an unreacted bond portion in which the number of strong siloxane bonds of the main component of the compound is not enough, so that it is distributed in the form of “dangling”. It is presumed that it easily penetrates into the soil when it is done, softens the infiltrated part, and eventually traps the radioactive material in the solidified interior.
  • the selection and use amount of the organometallic catalyst used as the catalyst the selection and use of the compound of Chemical Formula 2 and / or Chemical Formula 3
  • the practitioner can prepare relatively freely, and there is an effect that it can be freely selected depending on the degree of contamination.
  • the most characteristic feature is that the drug used captures radioactive pollutants and does not easily flow out depending on water or the like, and the trapping time can be maintained. Therefore, the contamination does not spread while the contaminated soil or the like is accumulated while capturing radioactive contaminants and transferred to another place.
  • the radioactivity protection by Japanese paper etc. becomes possible by making the chemical
  • the above-mentioned drug mixed with tungsten powder or molybdenum powder is applied or impregnated on Japanese paper, copy paper, Tyvek, the above-mentioned tungsten powder molten drug is applied to prevent the scattering of soil surface particles.
  • the radiation shielding rate (reduction rate) in comparison with the impregnated comparative reference sample “No. 0 Sat” shows an excellent radiation shielding effect of 23.8% to 52.4%.
  • the radiation reduction rate (shielding rate) in comparison with the collected soil (620 CPM) before impregnation with the liquid agent is a maximum of 48.4% to 67% as shown in “Radiation shielding rate with collected soil” in the above table. It has an excellent radiation shielding effect of .7% and has an excellent effect as a radiation shielding agent.
  • a paper material and a fiber material laminated by applying and impregnating the above-mentioned agent mixed with tungsten powder are a pure tungsten plate having the same thickness. Equivalent or 1.5 times the gamma ray shielding effect of tungsten plate, not only the liquid agent to be coated and impregnated functions as a radiation shielding agent, but also the paper material and fiber material itself impregnated and impregnated should be used as a radiation shielding material Can do.
  • a paper material coated with and impregnated with the above-mentioned agent mixed with tungsten fine powder a transcendent shielding paper A in which a plurality of fiber materials are laminated (in Example 8, 17 sheets are laminated) and boric acid ((H3BO3) 99.5%) Transcendental shielding paper B mixed with the above)) (in Example 8, the same 17 sheets laminated) has a neutron radiation shielding effect.
  • Figure 1 is a 200x magnified photograph of the surface of Japanese paper before applying the liquid agent.
  • Fig. 2 is a 200x magnified photograph of the surface of Japanese paper after the application of the "Super Transcendent + Tungsten (3.5 ⁇ m powder)"
  • FIG. 3 is an enlarged cross-sectional photograph of the 200 ⁇ Japanese paper.
  • Examples of the agent used for carrying out the prevention of scattering and decontamination / protection of radioactively contaminated soil according to the present invention include, for example, curing and solidifying by the action of a catalyst in a silane-based liquid containing a compound represented by Chemical Formula 1 as a main component.
  • Use possible drugs in Chemical Formula 1, R 1 , R 2 , R 3 and R 4 may be the same or different, each being hydrogen or an alkyl group having 1 to 4 carbon atoms)
  • Examples of the solidifying agent for radioactively contaminated soil and the agent used for carrying out the method for preventing surface scattering and decontamination / protection according to the present invention include, for example, among four substituents of silicon atoms as shown in Chemical Formula 1 Infiltrate by spraying on the contaminated soil surface with a compound containing one substituted with a non-hydrolyzable substituent as a repeating unit, solidify the soil surface, and capture radioactive material scattered on the soil surface In addition to preventing re-scattering, the solidified soil surface is scraped to make it possible to decontaminate radioactive materials.
  • the raw material (monomer) for obtaining the compound of Chemical formula 1 is relatively inexpensive. Therefore, it is sufficient to use the chemical formula 1 compound without using an expensive so-called silane coupling agent. It is possible to form solidified with the above organic properties and with sufficient strength. Even when transporting the scraped surface soil to other places, the radioactivity trapped inside The substance does not leak out.
  • the use of the compound represented by Chemical Formula 1 as a chemical used for carrying out the prevention of scattering and the decontamination / protection of the radioactively contaminated soil according to the present invention is extremely excellent.
  • medical agent which has the compound shown by Chemical formula 1 as a main component is sprayed on the contaminated soil surface where the radioactive substance scattered the chemical used to carry out the prevention of scattering of radioactively contaminated soil and decontamination / protection according to the present invention. In addition, it is cured and solidified by the action of a catalyst.
  • R 1 , R 2 and R 3 in Chemical formula 1 may be the same or different and are each hydrogen or an alkyl group having 1 to 4 carbon atoms, and n is preferably 2 to 10.
  • a compound in which n is 11 or more
  • the numerical value of n should not be interpreted restrictively.
  • the compound represented by Chemical Formula 1 include methyltrimethoxysilane, ethyltrimethoxysilane, propyltrimethoxysilane, butyltrimethoxysilane, methyltriethoxysilane, ethyltriethoxysilane, propyltriethoxysilane, butyltrimethoxysilane. Examples thereof include condensates such as ethoxysilane, methyltripropoxysilane, and ethyltripropoxysilane.
  • the compound of Chemical Formula 1 may be a product obtained by condensing only one kind of such monomers, or may be a product obtained by condensing two or more kinds of the above exemplified monomers.
  • the primary role of the non-hydrolyzable substituent (R 4 ) in the compound of Chemical Formula 1 is to provide flexibility to the soil surface, but at the same time, to impart water repellency to the soil surface.
  • R 4 may be an alkyl group.
  • the organic substituent has an organic property, that is, water repellency increases as the number of carbon atoms increases. However, when the carbon number is too large, distortion occurs in the soil surface due to steric hindrance and causes a decrease in strength of the film. Accordingly, the number of carbon atoms in the alkyl group and the type / amount of each monomer constituting the compound (condensate) of Chemical Formula 1 can be determined by conducting preliminary production tests while referring to the examples of the present specification.
  • imparting water repellency to the soil surface can also be achieved by adding a compound of Chemical Formula 2 or Chemical Formula 3, which will be described later, and therefore it is essential that R 4 in the compound of Chemical Formula 1 is an alkyl group. is not.
  • a commonly used catalyst can be used without any particular limitation.
  • an acid catalyst hydrochloric acid, nitric acid, sulfuric acid, phosphoric acid, formic acid or acetic acid
  • the base catalyst include ammonia, tetramethylammonium hydroxide, 2-hydroxyethyltrimethylammonium hydroxide, ethanolamine, diethanolamine, and triethanolamine.
  • the chemical used for carrying out the prevention of scattering and the decontamination / protection of the radioactively contaminated soil according to the present invention thus contains the compound of Chemical Formula 1, the catalyst and the reaction water.
  • the compound of Chemical Formula 1 In normal use, there is no particular problem. However, when this is stored for a long period of time, there is a problem that the drug is easily gelled by the reaction water.
  • organometallic compound When an organometallic compound is mixed with the compound of Chemical 1 to make a drug and sprayed onto the contaminated soil surface, moisture on the soil surface or inside or moisture in the air (humidity) is sucked and the organometallic compound hydrolyzes itself. At this time, a network is formed with the compound of chemical formula 1, and the chemical compound of chemical formula 1 is cured and solidified.
  • medical agent used in order to implement scattering prevention of the radioactively contaminated soil which concerns on this invention, and decontamination / protection what contains titanium, zircon, aluminum, or tin can be illustrated, for example.
  • tetrapropoxy titanate tetrabutoxy titanate, tetrapropoxy zirconate, tetrabutoxy zirconate, tripropoxy aluminate, aluminum acetylacetonate, dibutyltin diacetate, dibutyltin dilaurate, etc.
  • tripropoxy aluminate aluminum acetylacetonate, dibutyltin diacetate, dibutyltin dilaurate, etc.
  • an organic solvent can be added.
  • the organic solvent used for this purpose include alcohols. More specifically, methanol, ethanol, propanol, isopropanol, butanol, pentanol, hexanol and the like can be exemplified. Also, the viscosity and drying rate of the drug can be adjusted by controlling the amount added.
  • glycols such as ethylene glycol, propylene glycol, diethylene glycol, polyethylene glycol, dipropylene glycol, polypropylene glycol, methoxyethanol, propoxyethanol, butoxyethanol, methoxypropanol, ethoxypropanol, propoxypropanol
  • an organic solvent having a high viscosity or boiling point such as cellosolves such as butoxypropanol, alone or in combination.
  • the alcohols may be added simultaneously with one or more organic solvents having a high viscosity or boiling point.
  • the same effect can be achieved not only by the organic solvent but also by a surfactant.
  • glycols and cellsolves described above may be introduced into a network of siloxane bonds formed by the condensation reaction of the compound of formula 1. Since glycols and cellsolves are organic, the introduction of them increases the organicity of the resulting soil surface, that is, the organicity of the solidified soil surface.
  • medical agent contains the said organometallic compound (for example, tetrabutoxy titanium etc.) as a catalyst, the chemical change of (1) and (2) in the following reaction 1 occurs.
  • Reaction formula 1 (1) Ti-OR + H2O ⁇ Ti-OH + ROH (2) Ti-OH + RO-Si ⁇ Ti-O-Si
  • the strength of the solidified soil surface is improved by generating Ti—O bonds in the solidified soil surface.
  • an organometallic compound is used as a catalyst, not only the reaction water does not need to coexist, but also the strength of the solidified soil surface can be improved and a thin film of a silane compound can be applied to each fine particle. It can be formed.
  • the compound of Chemical Formula 2 added for such a purpose is a compound consisting of 4 substituents, in which 3 are hydrolyzable substituents and the remaining 1 is non-hydrolyzable substituents.
  • R 5 , R 6 and R 7 may be the same or different and each is a monomer comprising hydrogen, an alkyl group having 1 to 10 carbon atoms or an alkenyl group, and R 5 O, R 6 O and The bond between R 7 O and Si is an oligomer composed of a siloxane bond, and R 8 may contain an epoxy group or a glycidyl group in its molecule, an alkyl group having 1 to 10 carbon atoms, an alkenyl group, or It is a phenyl group.
  • Specific examples of the compound represented by Chemical Formula 2 include vinyltrimethoxysilane, phenyltrimethoxysilane, ⁇ - (methacryloxypropyl) trimethoxysilane, ⁇ -glycidoxypropyltrimethoxysilane, aminopropyltrimethoxysilane, ⁇ - (3,4 epoxy cyclohexyl) ethyltrimethoxysilane, vinyltriethoxysilane, phenyltriethoxysilane,-(methacryloxypropyl) triethoxysilane, ⁇ -glycidoxypropyltriethoxysilane, aminopropyltriethoxysilane, Examples thereof include vinyltris ( ⁇ methoxyethoxy) silane and the like, and a condensate of about 2 to 10 molecules thereof.
  • the compound of Chemical Formula 2 may be two or more of such monomers.
  • a compound obtained by condensing two or more of these monomers may be used.
  • the chemicals added with chemical compound 3 can be used to improve the organic properties of chemical compound 3 compared to the coating material produced without using chemicals. It is possible to increase the properties such as organic properties.
  • the compound of Chemical formula 3 is a compound consisting of four substituents, two of which are hydrolyzable substituents and the other two of which are non-hydrolyzable substituents.
  • R 9 and R 11 may be the same or different and each is a monomer comprising hydrogen, an alkyl group having 1 to 10 carbon atoms or an alkenyl group, and R 9 O, R 11 O and Si
  • the bond is an oligomer composed of a siloxane bond
  • R 10 and R 12 are an alkyl group, alkenyl group or phenyl group having 1 to 10 carbon atoms which may contain an epoxy group or a glycidyl group in the molecule. .
  • Specific examples of the compound represented by Chemical Formula 3 include dimethyldimethoxysilane, dimethyldiethoxysilane, diethyldimethoxysilane, diethyldiethoxysilane, diphenyldimethoxysilane, diphenyldiethoxysilane, methylvinyldimethoxysilane, and methylvinyldiethoxysilane. And a condensate of about 2 to 10 molecules thereof.
  • the compound of Chemical Formula 3 may be two or more of these monomers, and also when two or more molecules of condensate are used, There may be.
  • the organicity of the soil surface to be solidified can be increased, but both chemical compound 2 and chemical compound 3 are used as the drug. If added, the organicity of the solidified soil surface can be further improved, and as a result, the solidification strength of the soil surface can be further improved.
  • the compound of Chemical formula 2 and / or the chemical compound of Chemical formula 3 can be added to the drug in a range generally not exceeding 50% with respect to the compound represented by Chemical formula 1, which is the main component of the drug. preferable. If the total addition amount of both exceeds this range, when sprayed, it does not bind well with the main component compound 1, and the strength of the solidified soil surface may be insufficient. It is. Therefore, in the case of actually adding the chemical compound 2 and / or chemical compound 3, it is assumed that the strength of the soil surface solidified depending on the amount added, and the examples in the present specification are used. While referring to it, it is preferable to carry out a preliminary production test or the like, clarify the range of the addition amount that can achieve the object, and minimize the addition.
  • the primary role of the non-hydrolyzable substituents (R 8 , R 10 , R 12 ) in the chemical compound 2 and chemical compound 3 is to give flexibility to the soil surface to be solidified.
  • these are organic substitutions such as alkyl groups, they also serve to impart water repellency to the soil surface to be solidified at the same time. Therefore, even if the soil surface cannot be shaved immediately after solidification, the radioactive material trapped inside by rainwater or the like does not leak out.
  • the number of carbon atoms of an organic substituent is too large, strain is generated on the soil surface solidified by steric hindrance, causing a decrease in strength. Accordingly, the number of carbon atoms of the organic substituent and the type / amount of each monomer constituting the compound (condensate) of Chemical Formula 2 and / or Chemical Formula 3 are preliminarily referred to with reference to Examples in the present specification. It is preferable to make a determination by performing an appropriate manufacturing test.
  • the siloxane bond with improved strength is also a so-called “hard” bond. Because of this “hardness,” the soil surface that has been solidified lacks flexibility, which may cause difficulties in scraping and transporting work. Therefore, the soil surface that has been solidified may sometimes require moderate flexibility.
  • sol-gel drugs generally used are tetraalkoxysilane (Si (OR) 4 ) and oligomers thereof as a starting material, but these are completely hydrolyzed.
  • Si (OR) 4 tetraalkoxysilane
  • oligomers thereof as a starting material, but these are completely hydrolyzed.
  • Si (OR) 4 tetraalkoxysilane
  • all four bonds of silicon atoms form a network of hard siloxane bonds, which are as hard as ceramics, but are not flexible and tend to collapse. Since there is a danger, it is more preferable to use a chemical comprising the above-mentioned chemical formula 1 and / or chemical formula 2 and / or chemical formula 3 as prevention of scattering and decontamination / protection of radioactively contaminated soil according to the present invention. is there.
  • the chemicals used for carrying out the prevention of decontamination and decontamination / protection of radioactively contaminated soil according to the present invention are compounds of chemical formula 1 in which one of the four substituents of the silicon atom is not hydrolyzed It is because it is made into the main component of a medicine.
  • the compound of Chemical formula 2 and the chemical compound of Chemical formula 3 which have one or two substituents which are not hydrolyzed, respectively.
  • MTM methyltrimethoxysilane condensate
  • ETM ethyltrimethoxysilane condensate
  • MTE methyltriethoxysilane condensate
  • the drug is divided into (a) no spraying, (b) 50 cc spraying, (c) 100 cc spraying, (d) 200 cc spraying, (e) 250 cc spraying, and at 10:00 am on May 16, 2011 Around 30 minutes, the drug was sprayed in the above amount with a sprayer and sprayed, and the radiation intensity of the compartment was measured.
  • the measurement was performed using a simple radiation measuring instrument “Hakarun (DX-200)” lent out free of charge as a school education support project by the Ministry of Education, Culture, Sports, Science and Technology.
  • the specifications of “Hakaru-kun (DX-200)” are as follows.
  • Table 3 shows the measurement of the radiation intensity of the section after removing the solidified surface in the sections (a) to (e) above. That is, after the measurement in Table 2 is completed, the soil surface of sections (a) to (e) is solidified, so the surface of the transplanting iron is cracked and cracked, and the tip of the transplanting iron is broken from the crack. And the solidified surface was removed.
  • the section surface of (a) is about 3 mm thick
  • the section surface of (c) is about 5 mm thick
  • the partition surface of (6) can be stripped off with a thickness of about 6 mm
  • the partition surface of (e) can be stripped with a thickness of about 8-10 mm.
  • the capture state of the radioactive substance trapped inside the solidified drug itself was verified.
  • the soil surface of the solidified soil was brought home, and the above solidification was conducted at the Polymer Research and Evaluation Center Tokyo Office of the Japan Science Research Evaluation Organization (Shigeru Nagakayama, 2-22-13 Yanagibashi, Taito-ku, Tokyo).
  • the soil was stored in a container, and 4 liters of water was poured into the container over 1 hour, and then the solidified state and radioactivity level of the soil were measured. Even after 4 liters of water was poured over 1 hour, no change was seen in the solidified state of the soil and there was no decrease in radioactivity level.
  • a drug (200B) prepared by adjusting the viscosity based on the No. 7 drug was prepared. Since this drug is referred to as trial drug 200B in the applicant company, it is displayed as drug 200B.
  • the preparation of the drug 200B is as follows.
  • Example 3 (2) Preparation of measurement samples In Example 3, as described above, 50 g of the soil surface was sampled at Koriyama City Sake Lid Park, and these were placed in a 3.2 g weight container. Samples (B to G) were prepared by spraying the above B to G chemicals on the soil. For comparison, a sample (A) in which no drug was sprayed was also prepared.
  • Example 4 the medicine C, the medicine D, the medicine E, and the medicine F created in Example 2 were each soaked in a 135 mm ⁇ 155 mm Japanese paper (weight 1.5 g) with a brush and dried sufficiently. A Japanese paper sample coated with these drugs C to D was placed on the comparative sample A, and the radioactivity level was measured from the sample. The results are shown in Table 6.
  • (a) shows the radioactivity level of Sample A without using any drug, and the level is 620 CPM.
  • the radioactivity on the sample is covered with Japanese paper impregnated with the above drugs C to D.
  • the radioactivity levels were reduced to 440 CPM, 304 CPM, 400 CPM, and 440 CPM, respectively, and radioactivity protection was confirmed.
  • Example 4 181 g of methyltrimethoxysilane, 50 g of methanol and 18 g of pure water were added and stirred sufficiently, and further 2 g of 61% nitric acid was added and heated and refluxed for 3 hours with stirring.
  • the alkoxysilane condensate MTM shown in No. 7 of Table 1 obtained by removing the methanol in the reaction vessel under reduced pressure (mainly 3 to 4 mer by gas chromatography analysis)
  • Isopropyl alcohol (IPA) 2.5 liters
  • 200 g of 100B is mixed with 20 g, 25 g, and 30 g of lead oxide (chemical formula Pb + PbO).
  • the drug B, the drug C, and the drug D are mixed with 25 g, 30 g, and 40 g of lead monoxide (chemical formula PbO), respectively.
  • Each was coated with a brush on 135 mm x 155 mm Japanese paper (weight 1.5 g), soaked into the Japanese paper, dried, and these chemicals C to D were coated on the above-mentioned comparative sample A, and from above The radioactivity level was measured (measurement results are shown in “Table 6”).
  • Example 4 since the chemicals used in Example 4 above are a mixture of lead suboxide (Pb + PbO) and lead monoxide (PbO), there are difficulties in using them directly in contact with the human body. Also, environmental and other impacts must be considered. Therefore, in place of the above lead suboxide and lead monoxide, a tungsten or molybdenum molten chemical was applied and impregnated on Japanese paper, copy paper, and Tyvek (registered trademark), and the same measurement was performed. The tungsten and molybdenum used were those manufactured by Toho Metals Co., Ltd., in the form of 3.5 ⁇ m powder and 3N standard (99.9% purity). Its physical properties are as follows.
  • the above-mentioned drug 200B is used as a translucent agent, and tungsten and molybdenum are mixed in a weight ratio of 1.5 times each to obtain “transcendental liquid agent + tungsten (3.5 ⁇ m powder)” and “transcendental liquid agent + molybdenum (3. 5 ⁇ m powder) ”solution, and this solution was applied to Japanese paper, copy paper, and Tyvex, respectively.
  • Tyvek registered trademark
  • the material and weight (10 cm ⁇ 10 cm) of each sample are organized as follows. On top of that, three sheets of the above-mentioned Japanese paper (10 cm ⁇ 10 cm), two sheets of copy paper (10 cm ⁇ 10 cm), and two sheets of tyvek (10 cm ⁇ 10 cm) are prepared. The sheet was coated and impregnated with a solution obtained by mixing 1.5 times the weight of tungsten (3.5 ⁇ m powder) with the translucent solution (200B), and each measurement material sample was added to the “No. 1 Japanese paper” sample, “No. .2 Washi ”,“ No.3 Washi ”,“ No.1 Copy Paper ”,“ No.1 Tyvek ”, and“ No.2 Tyvek ”Samples. The liquid agent (200B) was coated and impregnated with a liquid agent obtained by mixing 1.5 times by weight of molybdenum (3.5 ⁇ m powder), and this was used as a “No. 2 copy paper” sample.
  • the “No. 0 Sat” sample is the “No. 1 Washi” sample, “No. 2 Washi” sample, “No. 3 Washi” sample, “No. 1 copy paper” sample, “No. 2” These are samples for comparison with the measured values of the “copy paper” sample, the “No. 1 tyvek” sample, and the “No. 2 tyvek” sample, and the above-mentioned July 7, 2011 used in Example 3 above.
  • the “SURVEY METER LUDLUM MODEL 14C” is also designed to meet the requirements of nuclear medicine, and can detect alpha rays, beta rays, and gamma rays from 0 to 200 MR / HR with one or more external GMs (Geiger Muller Detector) or a scintillation detector, which has the following specifications.
  • CPM count per minute or count per minute
  • the measured value of the comparative reference sample “No. 0 Sat” sample was 420 CPM, and further, each measurement data sample “No. 1 Japanese paper” sample, “No. 2 By placing ⁇ Washi '' sample, ⁇ No.3 Washi '' sample, ⁇ No.1 copy paper '' sample, ⁇ No.2 copy paper '' sample, ⁇ No.1 Tyvek '' sample, ⁇ No.2 Tyvek '' sample, It was found that each had a radiation shielding effect such as 200 CPM to 320 CPM.
  • the above table X is a comparison with 420 CPM of the “No. 0 soil” sample, but the “No. 0 soil” sample prevents the scattering of soil particles during the measurement as described above.
  • the above-mentioned “Transcendent (50 g) + Tungsten (3.5 ⁇ m powder) (75 g)” was applied and solidified, and originally, on July 7, 2011, Koriyama-shi Sakeku Park (Fukushima Prefecture) The soil is collected in Fukasawa, Koriyama City.
  • a direct measurement of this soil is 620 CPM (see Sample A), as shown in Table 5 of Example 3 above, which is the above-mentioned “transluent (50 g) + tungsten (3.5 ⁇ m powder) ( 75 g) ”is reduced to 420 CPM by applying and solidifying, and further, by placing each sample thereon, it can be known that the measurement results of 200 CPM to 320 CPM are obtained.
  • the radiation shielding rate (reduction rate) in comparison with the comparative reference sample “No. 0 Sat” shows an excellent radiation shielding effect of 23.8% to 52.4%.
  • the radiation reduction rate (shielding rate) in comparison with the collected soil (620 CPM) before the coating impregnation of the maximum is 48.4% to 67.67 as shown in “Radiation shielding rate with collected soil” in the above table. It has a radiation shielding effect of 7%.
  • Fig. 1 is a 200x magnified photograph of the surface of Japanese paper before application of the liquid agent
  • Fig. 2 is a magnified photograph of the surface of the 200 paper of Japanese paper after application of the "translucent agent + tungsten (3.5 ⁇ m powder)”
  • Fig. 3 is a magnification of 200x. It is a Japanese paper enlarged cross-sectional photograph. In any case, it can be known that the liquid agent penetrates to the surface of the Japanese paper and the inside of the cross section.
  • Example 5 the “translucent agent + 3N tungsten (3.5 ⁇ m powder)” solution used in Example 5 was applied to glass fiber (manufactured by NICHIAS), kraft paper, Japanese paper, and each sample was cut into 15 cm ⁇ 17 cm. Each sample was prepared by stacking 16 sheets and fixing with tape. For each sample, methyltrimethoxysilane, methanol, pure water, and nitric acid used in Example 5 above were added, and after completion of the heating and refluxing reaction, methanol was removed and the alkoxysilane condensate MTM obtained by isopropyl was added to isopropyl.
  • the sample coated and impregnated with glass fiber is called “W + glass fiber sample”
  • the sample coated and impregnated on the kraft paper is called “W + craft paper sample”
  • the sample coated and impregnated on the same paper is called “W + Japanese paper sample”.
  • “Sample No.”, “Sample Name”, and “Thickness (mm)” of each sample are as follows.
  • Measurement location Cobalt 60 irradiation room, Faculty of Engineering, Nagoya University ⁇ Measurement date: 2011 / ll / 28 (Monday), 12/2 (Friday), 12/5 (Monday): 10.00-16.00 ⁇ Measurement equipment: Co-60 irradiation device / Flicke dosimeter ⁇ Measurement purpose: Measure the radiation shielding rate of the sample ⁇ Use source: Co-60 ⁇ Measurement method: A lead block is constructed 30cm from the radiation source. A sample is attached to the hole of the block and the dose of ⁇ -ray is measured.
  • Irradiation time 60 [min] x 3 times per sample
  • Evaluation method / evaluator Based on the evaluation of Shigefumi Imai, the person in charge of irradiation / irradiation room management at the Cobalt 60 irradiation room at Nagoya University, using a Flicke dosimeter.
  • Samples used Samples made by applying a liquid to each sample.
  • Reference value When the sample is not installed, measure the dosimeter away from the irradiation window by the thickness of the sample. Measurement is one sample per day. The order of measurement was as follows.
  • sample “W + glass fiber” has a numerical value that is almost the same (98%) as the W plate having the same thickness.
  • Sample “W + kraft paper” has a numerical value of 150% higher than a W plate of equivalent thickness.
  • the sample “W + Japanese paper” obtained a numerical value slightly inferior (81%) to the W plate having the same thickness.
  • the gamma ray shielding according to this measurement is performed by laminating 16 samples of glass fiber impregnated with the above liquid agent, and ⁇ -ray shielding of a tungsten plate having a thickness of only 4.1 mm and an equivalent thickness.
  • the liquid agent is effective as a radiation ( ⁇ -ray) shielding agent, and a paper material or a fiber material impregnated with this liquid agent has a very excellent effect as a radiation ( ⁇ -ray) shielding material.
  • Example 2 was carried out by spraying the drug on the soil surface to prevent re-scattering of radioactive substances on the soil surface and decontamination of the soil surface, but this was limited to the soil surface only. For example, even if it is a concrete surface, it is possible to prevent re-scattering of radioactive materials, as well as decontamination of radioactive materials, for example, by spraying cryogenic dry ice particles etc. It is clear that the surface can be peeled off and has a certain effect within the range of the decontamination evaluation (part 2).
  • scattering prevention and decontamination / protection of radioactively contaminated soil according to the present invention are not limited to the soil surface, and as long as the surface properties are allowed, the prevention of re-scattering of radioactive materials on the surface of any material It can also be applied to decontamination / protection.
  • the “transcendent solution (200B) + 3N tungsten (3.5 ⁇ m powder)” solution used in Example 5 above was applied to kraft paper, and the applied kraft paper was cut into 22 cm ⁇ 22 cm sample A (hereinafter “transcendence”). Also referred to as “shielding paper A”. Specifically, 750 g of 3N tungsten (3.5 ⁇ m powder) is mixed with 500 g of the translucent agent (200B), and this is applied to kraft paper having a thickness of 95.3 ⁇ m and a weight of 70 g / m 2 . The coated kraft paper was cut into 22 cm ⁇ 22 cm to obtain Sample A.
  • a tungsten plate having a thickness of 1 mm ⁇ 26.5 cm ⁇ 33.5 cm and a weight of 1759 g was prepared.
  • 22 cm ⁇ 22 cm and a weight of 970 g are measured
  • 22 cm ⁇ 22 cm and a weight of 1040 g are measured.
  • the neutron beam shielding rate was measured.
  • the measurement method is a height of 1 m from the floor, the distance from the source to the measurement center of the detector is 25 cm, and there is a case where there is no sample in between, and the dose rate is shielded from the average value measured 10 times each. The rate was determined.
  • the tungsten plate had a thickness of 1 mm, 26.5 cm ⁇ 33.5 cm, and a weight of 1759 g.
  • the weight of the measurement sample was 22 cm ⁇ 22 cm (970 g).
  • a weight (970 g) equivalent to a 22 mm ⁇ 22 cm 1 mm thick tungsten plate A measurement sample was obtained by stacking 17 sheets so as to be bundled.
  • the above transcendental shielding paper B 17 sheets of the same sheet were stacked and bundled, and the weight thereof was 1040 g.
  • the dose rate and shielding rate for the neutron source are as follows.
  • the dose rate when there was no sample was 27.4 ⁇ 0.4 ⁇ Sv / hour, and the shielding rate was obtained by (1 ⁇ with sample / without sample) ⁇ 100.
  • the dose rate of the neutron source with a 1 mm thick tungsten plate is 27.0 ⁇ 0.5 ( ⁇ Sv / hr), and the shielding rate is 1.5%
  • the transcendent shielding paper In A the dose rate is 25.9 ⁇ 0.5 ( ⁇ Sv / hour) and the shielding rate is 5.5%
  • the dose rate in the transcendent shielding paper B the dose rate is 25.04 ⁇ 0.4 ( ⁇ Sv / hour) and the shielding rate is 7.%. 3% was obtained.
  • the measurement sample A is obtained by coating and impregnating a fiber material such as paper with a solution in which tungsten powder is added while stirring and adding a catalyst to an alkoxysilane solution of an organosiliconized material evolved by using a sol-gel method.
  • the contained component alkoxysilane reacts with the moisture in the paper or in the air to initiate polycondensation reaction to silicon, and the contained component silicic acid is a glassy basic skeleton.
  • a siloxane bond occurs.
  • the vitreous liquid is soaked into the surface of the fine powder of tungsten existing between each fiber of paper or the like by capillarity, the gap, and every corner of the paper fiber to be polymerized. It becomes.
  • the silane-based thin film containing tungsten fine powder and the paper fiber are formed integrally between the paper fibers, and the silane-based liquid also contains organic matter, so the bonded surface layer is moderately flexible. It has mechanical properties that have both properties and water repellency.
  • the measurement sample B (transcendent shielding paper B) is prepared by adding fine powder of boric acid to a solution obtained by adding a catalyst to an alkoxysilane solution to the tungsten fine powder, and stirring the resulting powder into a fiber material such as paper. It is coated and impregnated.
  • radiation such as ⁇ -rays, ⁇ -rays, ⁇ -rays, and X-rays
  • the energy it holds is given to the substance, causing interactions at the atomic level such as ionization and excitation.
  • the transcendent shielding paper A and transcendental shielding paper B detailed knowledge is not clear, but the silane compound and glass in the coated and impregnated fiber are not clear.
  • fine tungsten powder Since fine tungsten powder is present in multiple layers in a multifaceted and superposed manner, the fine tungsten powder causes reflection, absorption, scattering, re-radiation, etc. of invading neutrons, which has a shielding effect. It is speculated that it is caused.

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Abstract

L'invention a pour objet un agent pour le durcissement et la solidification d'un sol contaminé radioactif, ledit agent permettant la rétention d'une substance contaminée radioactive, qui sinon se disperserait facilement et, dans le cas où le sol de surface doit être enlevé, rendant l'enlèvement facile. L'invention a également pour objet un procédé pour la prévention de la dispersion d'une substance radioactive, la décontamination et la protection. L'agent de durcissement et de solidification selon l'invention est à base de silane et durcit et solidifie un sol de surface contaminé radioactive, ledit agent de durcissement et de solidification comprenant un composé représenté par la formule chimique (1) comme composant principal conjointement avec un catalyseur pour le durcissement et la solidification de celui-ci. Dans la formule (1), R1, R2, R3 et R4 peuvent être identiques ou différents et représentent chacun un atome d'hydrogène ou un groupe alkyle en C1-4.
PCT/JP2012/067554 2011-08-01 2012-07-10 Agent pour le durcissement et la solidification du sol de surface contaminé radioactif, agent bloquant les rayonnements et procédé pour la prévention de la dispersion de substance radioactive à partir d'une surface, la décontamination et la protection Ceased WO2013018512A1 (fr)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP5321992B1 (ja) * 2011-08-17 2013-10-23 独立行政法人農業・食品産業技術総合研究機構 汚染土壌表層の除去工法
WO2022069739A1 (fr) * 2020-10-01 2022-04-07 Caradonna Emiliano Procédé de traitement d'eaux usées liquides radioactives et appareil pour la mise en oeuvre du procédé

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JPS6071996A (ja) * 1983-09-29 1985-04-23 チッソ株式会社 放射線防禦材用重金属系組成物
JPS61241699A (ja) * 1985-04-18 1986-10-27 東レ・ダウコーニング・シリコーン株式会社 γ線遮蔽用オルガノポリシロキサン組成物
JPH045207A (ja) * 1990-04-23 1992-01-09 Nichiban Kenkyusho:Kk 抗菌・消臭材
JPH0692758A (ja) * 1991-12-20 1994-04-05 Toyo Ink Mfg Co Ltd 水性有機珪素系組成物
WO2002044277A1 (fr) * 2000-12-01 2002-06-06 Kanebo, Limited Resine moulee anti-radiations
JP2007271539A (ja) * 2006-03-31 2007-10-18 Nippon Tungsten Co Ltd 樹脂タングステン複合材料
JP2012042300A (ja) * 2010-08-18 2012-03-01 Sanyo Chem Ind Ltd 放射能拡散防止用組成物
JP2012112797A (ja) * 2010-11-25 2012-06-14 Toshiba Corp 放射性廃液の処理方法及び処理装置

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Publication number Priority date Publication date Assignee Title
JPS6071996A (ja) * 1983-09-29 1985-04-23 チッソ株式会社 放射線防禦材用重金属系組成物
JPS61241699A (ja) * 1985-04-18 1986-10-27 東レ・ダウコーニング・シリコーン株式会社 γ線遮蔽用オルガノポリシロキサン組成物
JPH045207A (ja) * 1990-04-23 1992-01-09 Nichiban Kenkyusho:Kk 抗菌・消臭材
JPH0692758A (ja) * 1991-12-20 1994-04-05 Toyo Ink Mfg Co Ltd 水性有機珪素系組成物
WO2002044277A1 (fr) * 2000-12-01 2002-06-06 Kanebo, Limited Resine moulee anti-radiations
JP2007271539A (ja) * 2006-03-31 2007-10-18 Nippon Tungsten Co Ltd 樹脂タングステン複合材料
JP2012042300A (ja) * 2010-08-18 2012-03-01 Sanyo Chem Ind Ltd 放射能拡散防止用組成物
JP2012112797A (ja) * 2010-11-25 2012-06-14 Toshiba Corp 放射性廃液の処理方法及び処理装置

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP5321992B1 (ja) * 2011-08-17 2013-10-23 独立行政法人農業・食品産業技術総合研究機構 汚染土壌表層の除去工法
WO2022069739A1 (fr) * 2020-10-01 2022-04-07 Caradonna Emiliano Procédé de traitement d'eaux usées liquides radioactives et appareil pour la mise en oeuvre du procédé
WO2022069053A1 (fr) * 2020-10-01 2022-04-07 Caradonna Emiliano Procédé de traitement d'eaux usées liquides radioactives et appareil pour la mise en œuvre du procédé

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