RADIATION-SCINTILLATED SHIELD AND MANUFACTURING METHOD OF RADIATION SHIELDING RESIN
20220308243 · 2022-09-29
Assignee
- Toshiba Energy Systems & Solutions Corporation (Kawasaki-shi, Kanagawa, JP)
- Toshiba Materials Co., Ltd. (Yokohama-shi, Kanagawa, JP)
Inventors
- Kohichi NAKAYAMA (Yokohama Kanagawa, JP)
- Koichi NITTOH (Yokohama Kanagawa, JP)
- Yukio SONODA (Kisarazu Chiba, JP)
- Yukihiro FUKUTA (Yokohama Kanagawa, JP)
Cpc classification
G21K4/00
PHYSICS
International classification
Abstract
According to an embodiment, a radiation-scintillated shield which attenuates an incident radiation, includes a shielding part containing an activator-added gadolinium compound as an aggregate. The activator uses the gadolinium compound as a base material and emits light when struck by the radiation. Consequently, it becomes possible to shield a γ-ray and a neutron with a thickness which is about the same as that of a conventional concrete shield of γ-ray shield, and to confirm leakage of radiation.
Claims
1. A radiation-scintillated shield which attenuates incident radiation, comprising a shielding part containing an activator-added gadolinium compound as an aggregate, wherein the activator uses the gadolinium compound as a base material and emits light when struck by the radiation.
2. The radiation-scintillated shield according to claim 1, wherein the shielding part is formed together with a transparent resin.
3. The radiation-scintillated shield according to claim 1, wherein the shielding part is used for attenatin a γ-ray and a low-energy neutron.
4. The radiation-scintillated shield according to any one of claim 1, wherein the gadolinium compound contains at least any one of gadolinium oxide, gadolinium gallium garnet, gadolinium oxysulfide, and gadolinium silicate.
5. The radiation-scintillated shield according to any one of claim 1, wherein the activator contains a rare-earth element.
6. The radiation-scintillated shield according to claim 5, wherein the rare-earth element includes at least any one of terbium, praseodymium, europium, and cerium.
7. The radiation-scintillated shield according to any one of claim 1, wherein the gadolinium compound and the activator are provided as a sintered compact thereof.
8. The radiation-scintillated shield according to claim 2, wherein a part of the transparent resin is arranged on an incident side of the radiation, or a density of the shielding part is made to have a gradient and a low-density portion is arranged on the incident side.
9. A manufacturing method of a radiation shielding resin formed of an activator-added gadolinium compound together with a transparent resin, the manufacturing method comprising: mixing an aggregate containing the gadolinium compound and the activator with resin in a container; and causing sedimentation of the aggregate with a large density to separate the mixture into an aggregate keeping layer and a resin layer.
Description
BRIEF DESCRIPTION OF THE DRAWINGS
[0018]
[0019]
[0020]
[0021]
[0022]
[0023]
[0024]
[0025]
[0026]
DETAILED DESCRIPTION
[0027] An object of an embodiment of the present invention is to enable to perform shielding of a γ-ray and a neutron with a thickness which is about the same as that of a conventional concrete shield of γ-ray shield, and to enable to confirm leakage of radiation.
[0028] According to an aspect of the present invention, there is provided a radiation-scintillated shield which attenuates incident radiation, comprising a shielding part containing an activator-added gadolinium compound as an aggregate, wherein the activator uses the gadolinium compound as a base material and emits light when struck by the radiation.
[0029] Hereinafter, a radiation-scintillated shield and a manufacturing method of a radiation shielding resin according to embodiments of the present invention will be described while referring to the drawings. Here, mutually the same parts or similar parts are denoted by common reference numerals, and overlapped explanation thereof will be omitted.
First Embodiment
[0030]
[0031] The radiation-scintillated shield 100 according to the present embodiment includes a concrete shielding part 10 as a shielding part 5. The concrete shielding part 10 includes an aggregate 11 and a cement portion 14.
[0032] The aggregate 11 is formed of a coarse aggregate 12 and a fine aggregate 13. Here, the coarse aggregate 12 is an aggregate in which particles each having a particle shape of 5 mm or more are included by 85% or more of the entire thereof, and the fine aggregate indicates one in which a particle diameter of each of all particles is 10 mm or less, and the particle diameter of 85% or more of all the particles is 5 mm or less.
[0033] Specifically, as the fine aggregate 13, one of a powder state is used. Further, the coarse aggregate 12 includes an aggregate with a large particle shape, an aggregate with a medium particle shape, and an aggregate with a relatively small particle shape, such as a large-size aggregate 12a, a medium-size aggregate 12b, and a small-size aggregate 12c.
[0034] A material of the aggregate 11 is a gadolinium compound. As the gadolinium compound, it is possible to use, for example, gadolinium oxide (Gd.sub.2O.sub.3: abbreviated as GO, hereinafter), gadolinium gallium garnet (Gd.sub.3Ga.sub.5O.sub.12: abbreviated as GGG, hereinafter), gadolinium oxysulphide (Gd.sub.2O.sub.2S: abbreviated as GOS, hereinafter), gadolinium silicate (Gd.sub.2SiO.sub.5: abbreviated as GSO, hereinafter), and the like. Here, a density of GO is 7.4 g/cm.sup.3, a density of GGG is 7.09 g/cm.sup.3, a density of GOS is 7.3 g/cm.sup.3, and a density of GSO is 6.7 g/cm.sup.3.
[0035] Gadolinium (Gd) being a rare-earth element is rare metal. Isotopes thereof that exist in the nature are six types of .sup.154Gd (2.18%), .sup.155Gd (14.80%), .sup.156Gd (20.47%), .sup.157Gd (15.65%), .sup.158Gd (24.84%), and .sup.160Gd (21.86%). Note that the numeric value within parentheses indicates a natural abundance. The .sup.160Gd becomes .sup.160Dy being a stable nuclide through β disintegration (half-life of 3.1×10.sup.19 years). The Gd isotopes other than that are stable nuclides.
[0036] A main reaction of Gd is (n, γ) reaction of absorbing the neutron and discharging the γ-ray. By each of (n, γ) reactions of .sup.154Gd, .sup.155Gd, .sup.156Gd, and .sup.157Gd, a stable nuclide of .sup.155Gd, .sup.156Gd, .sup.157Gd, and .sup.158Gd is generated respectively. In the case of .sup.158Gd, .sup.159Gd generated from .sup.158Gd by the (n, γ) reaction is turned into terbium 159 (.sup.159Tb) being a stable isotope, in accordance with β disintegration. By this disintegration, β-rays of 970.6 keV (62%), 912.6 keV (26%), 607.09 keV (12%), and 622.42 keV (0.31%) are discharged. Further, γ-rays of 363.55 keV (11.4%), 58 keV (2.15%), 348.16 keV (0.234%), and 226.16 keV (0.215%) are discharged.
[0037] In particular, each of 157Gd and 155 Gd having a large reaction cross section in a thermal neutron region discharges a neutron capture γ-ray of 8 MeV through the (n, γ) reaction. A discharge mode of this γ-ray can be roughly classified into two, which are a continuous spectrum and a discrete spectrum. Almost all (93.8%) of the discharge mode of γ-ray is the continuous spectrum, which is a spectrum in which, from an unstable compound nucleus to a stable ground level, single energy of 8 MeV is not discharged but a discharge ratio ranging from high energy to low energy becomes large. On the other hand, in the discrete spectrum, γ-rays with high energy such as 5.62 MeV+2.25 MeV (1.3%), 5.88 MeV+1.99 MeV (1.6%), 6.74 MeV+1.11 MeV (0.02%), and 7.87 MeV (0.02%) are discharged, but a proportion thereof is small to be 6.2%.
[0038] Note that a resonance region of the neutron capture reaction described above is in a range of about 10 eV to about 3 keV in the case of .sup.154Gd, it is in a range of about 2 eV to about 200 eV in the case of .sup.155Gd, it is in a range of about 30 eV to about 2 keV in the case of .sup.156Gd, and it is in a range of about 3 eV to about 300 eV in the case of .sup.157Gd. Therefore, an energy region including a thermal neutron region which is so-called 1/V region, and a region up to several KeV including a resonance region higher than the above energy region, for example, a region up to 3 keV, will be collectively referred to as a low-energy region in this embodiment.
[0039] The shielding performance with respect to the γ-ray (including the X-ray) depends on not only the density but also the atomic number Z. The number n of exponentiation is different depending on a reaction situation (photoelectric effect, Compton scattering, electron pair creation). The atomic number of gadolinium is 64 and the atomic number of iron is 26, and thus Z of gadolinium is about 2.5 times that of iron, so that it becomes important to use gadolinium. Further, regarding a specific weight as well, a specific weight of a conventional example produced as a radiation shield is about 3.5. On the other hand, a specific weight of a concrete shielding part 10 in which all of the aggregates are made of GOS is 4.9 or more, which is larger than that of a shield produced by using an iron and steel material as an aggregate.
[0040] Besides, an activator using a gadolinium compound selected from these as a base material, is added. As the activator, a rare-earth element is used. Among rare-earth elements, for example, praseodymium (Pr), terbium (Tb), europium (Eu), cerium (Ce), and the like are particularly preferable.
[0041] Each of the fine aggregate 13 and the coarse aggregate 12 is powder made by adding the activator to the aforementioned gadolinium compound, or a sintered compact made by firing the powder. Note that, the firing is performed through HIP (Hot Isostatic Pressing) or hot pressing.
[0042] A proportion of the activator to be added to the gadolinium compound is 0.001 mol % (10 ppm) to 50 mol %. If the proportion of the activator is less than 0.001 mol %, the light emission effect has no significance. If the proportion of the activator exceeds 50 mol %, the light emission effect has no significance due to concentration quenching, and further, since the proportion of gadolinium becomes small, the shielding effect has no significance. Further, the proportion of the activator to be added to the gadolinium compound is preferably 0.1 mol % to 10 mol %.
[0043] Before the firing into the ceramic or sintered compact, the particle size distribution is broadened, or after the firing into the ceramic or sintered compact, grinding is performed to broaden the particle size, to thereby obtain the fine aggregate 13 and the coarse aggregate 12.
[0044] Generally, a coarse aggregate and a fine aggregate used for concrete are gravel and sand. The concrete is formed of cement, water, a coarse aggregate, a fine aggregate, and an admixture. The coarse aggregate has the highest volume proportion, the fine aggregate has the second highest volume proportion, and the cement, the water, and the admixture exist in gaps of these aggregates.
[0045] In the concrete shielding part 10 of the present application, the materials of the coarse aggregate and the fine aggregate of the general concrete are replaced with the coarse aggregate 12 and the fine aggregate 13 molded from the gadolinium compound and the activator. Therefore, the proportion of the cement 14, the water, the coarse aggregate 12, the fine aggregate 13, and the admixture, processes such as kneading and solidification, and the like, are similar to those of normal concrete.
[0046] Note that in the shielding part 5, it is also possible to configure such that the density of the aggregate 11 is monotonously increased toward a direction in which the radiation 1 transmits, namely, the density of the aggregate 11 is made to have a gradient in the direction in which the radiation 1 transmits, and a low-density portion is arranged on the incident side.
[0047] Next, physical characteristics of the aggregate in the radiation-scintillated shield according to the first embodiment will be described.
[0048]
[0049] Density: 7332 kg/m.sup.3
[0050] X-ray absorption coefficient: 7240 m.sup.−1 (at 6.0 KeV) [0051] 3380 m.sup.−1 (at 8.0 KeV)
[0052] Refractive index: 2.22 (at 633 nm)
[0053] Micro Vickers hardness: 4420 MPa (load 1.0 kg)
[0054] Linear expansion coefficient: 8.8×10.sup.−6/° C. (at 23° C. to 385° C.)
[0055] Heat conductivity: 13.5 W/(m.Math.K) (at 29° C.)
[0056] Electric conductivity: 4.68×10.sup.−13 Q.sup.−1.Math.m.sup.−1
[0057] Specific heat: 0.287 (at 30° C.)
[0058] The density which is important for shielding the γ-ray is 7332 kg/m.sup.3, which is far larger than that of materials such as B and Li which are conventionally used for the neutron absorbing material, and is close to the density of iron and steel, and the like.
[0059] The linear expansion coefficient is 8.8×10.sup.−6/° C., which is sufficiently smaller than 1.0×10.sup.−5/° C., which is a linear expansion coefficient of iron and concrete.
[0060] The other physical characteristics also have no special points in particular.
[0061]
[0062] In the case of
[0063]
[0064] In the case of
[0065] The cases of using GOS as the base material and Pr and Tb for the activators are exemplified by using
[0066] The light emission phenomenon in this case is caused in a process in which when the entire GOS containing Gd atoms configuring GOS is irradiated with the radiation 1, carriers (electron-holes) are generated, the activator is excited, and transition to a low-energy level is caused.
[0067] Peaks capable of being detected are different depending on a sensitivity region of a light detector (including a camera), but any of the peaks can be detected by a normal light detecting unit. Regarding the detection of light, in order to secure an S/N ratio, it is preferable to use a band filter which allows only a region including a peak wavelength to be a detection target to pass therethrough. Here, the band filter may be an optical filter, or it is also possible to use an electrical band filter after photoelectric conversion.
[0068]
[0069] A curve C1 indicated by a solid line indicates a case of GOS. A curve C2 indicated by a dotted line indicates a case of Lead. A curve C3 indicated by a broken line indicates a case of Iron. Further, a curve C4 indicated by an alternate long and short dashed line indicates a case of B.sub.4C.
[0070] Among these substances, lead having the largest atomic number Z of 82, causes the largest attenuation of the γ-ray. On the other hand, the atomic number Z of Gd is large to be 64, which provides a high shielding effect of the γ-ray, and GOS being a compound of Gd, O, and S, exhibits the attenuation effect which is about the same as that of iron. The B.sub.4C having the effect of shielding the neutron, has the smallest attenuation effect of the γ-ray.
[0071] Among the elements, Gd has the largest reaction cross section with respect to the thermal neutron. Among the above-described natural isotopes of Gd, .sup.157Gd and .sup.155Gd, in particular, have the reaction cross sections of 66 times and 15.8 times, respectively, larger than the reaction cross section of .sup.10B, at the thermal neutron energy of 0.0253 eV of neutron energy. Further, as described above, at the energy from 100 eV to the vicinity of 1 KeV, not only .sup.157Gd and .sup.155Gd but also the other Gd isotopes have a plurality of resonance absorption peaks, and have a cross section larger than that of .sup.10B.
[0072] As described above, the main reaction of Gd with the neutron is different from the reaction of boron, and is the (n, γ) reaction of reacting with the neutron and discharging the γ-ray. The reaction of boron is (n, α) reaction, in which .sup.7*Li is generated, and in a process of turning into .sup.7Li, a prompt γ-ray of 478 KeV is discharged. On the other hand, in the case of Gd, .sup.155Gd, .sup.156Gd, .sup.157Gd, and .sup.158Gd which are respectively generated by the (n, γ) reactions of .sup.154Gd, .sup.155Gd, .sup.156Gd, and .sup.157Gd, respectively, are stable isotopes, and secondary products which discharge β-rays or γ-rays in accordance with disintegration are not generated.
[0073] As described above, GOS has not only the above-described shielding effect with respect to the neutron but also an attenuation effect with respect to the γ-ray which is about the same as that of iron.
[0074]
[0075] When the defect portion 100d is generated in the radiation-scintillated shield 100 as above, a light emission intensity of the shield surface on opposite side of radiation source 100r becomes large partially, and thus it is possible to confirm the defect. Further, this confirmation can be performed even remotely as long as light can be visually recognized.
[0076]
[0077]
[0078] In order to detect light from shield surfaces on opposite side of radiation source 100m, 100n, and 100r of the concrete shielding parts 10a, 10b, and 10c, respectively, a first light detector 32a, a second light detector 32b, and a third light detector 32c are respectively provided.
[0079] In a manner as above, by measuring the light emission intensities at the shield surfaces on opposite side of radiation source 100m, 100n, and 100r along the direction in which the radiation 1 transmits, it is possible to check the attenuation effect of the radiation 1.
[0080] As described above, according to the radiation-scintillated shield 100 according to the present embodiment, it is possible to obtain the following features and effects.
[0081] Firstly, there can be cited a point that the radiation-scintillated shield 100 emits light when struck by the gamma (X)-ray and the neutron in particular in the thermal neutron region. The radiation 1 can be detected by the light detector. Therefore, it becomes possible to visually recognize the leaked radiation remotely, for example, in a case where the radiation 1 leaks to the outside of a radiation shield which is intended for biological shielding. Consequently, it is possible to recognize a place where the leakage of radiation 1 occurs, and even the intensity of the radiation 1. On the other hand, when a radiation detector is used, it is not possible to specify the place where the leakage of radiation 1 occurs as described above, unless each radiation intensity of each point of a surface of a radiation shield is measured.
[0082] Secondly, there can be cited a point that the aggregate 11 of the radiation-scintillated shield 100 has weight which is about the same as that of the conventional concrete shield for γ-ray shielding, and it has both the function of shielding the neutron and the function of shielding the gamma (X)-ray. Specifically, with a concrete thickness which is nearly equal to or smaller than that of the conventional concrete (including mortar as well) of γ-ray shield, it is possible efficiently shield both the neutron and the gamma (X)-ray.
[0083] Thirdly, there can be cited a point that in the radiation-scintillated shield 100, an alkali-aggregate reaction being one of deterioration phenomena of general concrete, is unlikely to occur. As the alkali-aggregate reaction, an alkali-silica reaction (ASR) and an alkali-carbonate reaction are known. These are reaction phenomena in which metal ions of sodium, potassium, and the like contained in cement are subjected to a chemical reaction with silica in the mineral of the aggregate, resulting in that abnormal expansion occurs, which causes cracks in the concrete. On the other hand, the aggregate 11 of the radiation-scintillated shield 100 according to the present embodiment has a characteristic that it is a harmless aggregate containing no substance which causes this alkali-silica reaction.
[0084] Fourthly, there can be cited a point that the aggregate 11 of the radiation-scintillated shield 100 is produced through the HIP treatment, and thus the aggregate 11 itself endures high-temperature and high-pressure states, and besides, a thermal expansion coefficient of the aggregate 11 is very small. Specifically, the linear expansion coefficient of GOS is 8.8×10.sup.−6/° C., which is sufficiently smaller than the linear expansion coefficient of iron and concrete of 1.0×10.sup.−5/° C. For this reason, there is a characteristic that fracture or crack due to the thermal expansion of the aggregate itself is unlikely to occur.
Second Embodiment
[0085]
[0086] The present embodiment is a modification of the first embodiment. Specifically, a radiation-scintillated shield 100a according to the present embodiment includes a concrete shielding part 10 similar to that of the first embodiment, as a shielding part 5, and it further includes a radiation shielding resin 20.
[0087] As illustrated in
[0088] The radiation shielding resin 20 includes an aggregate 21 and a resin portion 24.
[0089] The aggregate 21 includes a coarse aggregate 22 and a fine aggregate 23. For a material of the aggregate 21, it is possible to use ceramic or sintered compact molded from a mixture of granules of a gadolinium compound and granules of an activator, in a similar manner to the aggregate 11.
[0090] The aggregate 21 exists unevenly on a downstream side of an incident direction of the radiation 1, in the radiation shielding resin 20, and it forms an aggregate keeping layer 20b together with resin. Further, a resin layer 20a is a layer composed only of resin, but the fine aggregate 23 may exist within a region of the resin layer 20a.
[0091]
[0092] First, an aggregate and resin are prepared for each of the aggregate 21 and the resin portion 24 (step S1). Note that for the resin portion 24, resin with a large content of paraffin or hydrogen is used. Further, as the resin, for example, a two-liquid-mixing type transparent resin with low viscosity and long curing time is used. For example, an amount of an epoxy resin is set to a proportion of about 1.5 to 2 times or more a volume capacity of a GOS piece. In a case where the curing time becomes long when the temperature is low, due to a relation with temperature, the curing time is set to be long by performing temperature control in a transition step.
[0093] Next, the aggregate whose volume ratio is half or less relative to a volume amount of the resin, is mixed with the resin and stirred (step S2). For example, a main agent of the first liquid and the light-emitting GOS piece are accommodated in a container, and then sufficiently stirred. Next, a curing agent of the second liquid is added.
[0094] Next, the container is vibrated, to thereby perform defoaming and deaeration of air and the like in the resin (step S3). The vibration of the container is performed by mounting the container on a vibration table, for example. Further, the deaeration can be performed by using, for example, a vacuum chamber. An environmental temperature of the container is set to a low-temperature state so as to decrease a curing speed of the epoxy resin.
[0095] Next, while keeping the vibration, sedimentation of the aggregate with a large density is caused, to thereby separate the mixture into the resin layer 20a and the aggregate keeping layer 20b (step S4). While a specific weight of the epoxy resin is about 1.1 to 1.4 g/cm.sup.3, the density of the GOS piece is 7.3 g/cm.sup.3 or more, so that when the curing is caused while vibrating the entire container, there is created a situation where the sedimentation of GOS piece is caused due to the difference in specific weight and the GOS piece is deposited densely on the lower side, and an upper part is formed substantially only of the transparent resin layer. Specifically, the resin layer 20a and the aggregate keeping layer 20b are vertically separated from each other with the resin layer 20a positioned above the aggregate keeping layer 20b. The resin layer 20a includes only the resin portion 24, or a part of the fine aggregate 23. The aggregate keeping layer 20b includes the aggregate 21 and the resin portion 24.
[0096] Next, the curing of resin is completed (step S5).
[0097] Note that it is also possible that in step S4, the sedimentation is not completely finished, and the resin is cured in the middle stage of the sedimentation. In this case, it is possible that, in the shielding part 5, the density of the aggregate 11 is monotonously increased in the direction in which the radiation 1 transmits, namely, the density of the aggregate 11 is made to have a gradient in the direction in which the radiation 1 transmits, to thereby arrange the low-density portion on the incident side.
[0098] As described above, according to the present embodiment, slowing-down fast neutron to a low-energy region including a thermal neutron region or a resonance region in an early stage makes it possible to accelerate the reaction between the low-energy neutron, and the aggregate 11 and the aggregate 21.
Other Embodiments
[0099] While the embodiments of the present invention have been described above, the embodiments have been presented by way of example only, and are not intended to limit the scope of the inventions.
[0100] Further, the characteristics of the respective embodiments may also be combined. Further, the embodiments can be embodied in a variety of other forms, and various omissions, substitutions and changes may be made without departing from the spirit of the inventions.
[0101] The accompanying claims and their equivalents are intended to cover such forms or modifications as would fall within the scope and spirit of the inventions.