WO2015008370A1 - 中性子吸収ガラス及びそれを用いた中性子吸収材料、並びにこれらを適用した溶融燃料の管理方法、溶融燃料の取り出し方法及び原子炉の停止方法 - Google Patents
中性子吸収ガラス及びそれを用いた中性子吸収材料、並びにこれらを適用した溶融燃料の管理方法、溶融燃料の取り出し方法及び原子炉の停止方法 Download PDFInfo
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- WO2015008370A1 WO2015008370A1 PCT/JP2013/069578 JP2013069578W WO2015008370A1 WO 2015008370 A1 WO2015008370 A1 WO 2015008370A1 JP 2013069578 W JP2013069578 W JP 2013069578W WO 2015008370 A1 WO2015008370 A1 WO 2015008370A1
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C9/00—Emergency protection arrangements structurally associated with the reactor, e.g. safety valves provided with pressure equalisation devices
- G21C9/02—Means for effecting very rapid reduction of the reactivity factor under fault conditions, e.g. reactor fuse; Control elements having arrangements activated in an emergency
- G21C9/033—Means for effecting very rapid reduction of the reactivity factor under fault conditions, e.g. reactor fuse; Control elements having arrangements activated in an emergency by an absorbent fluid
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C12/00—Powdered glass; Bead compositions
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/04—Glass compositions containing silica
- C03C3/062—Glass compositions containing silica with less than 40% silica by weight
- C03C3/064—Glass compositions containing silica with less than 40% silica by weight containing boron
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/04—Glass compositions containing silica
- C03C3/062—Glass compositions containing silica with less than 40% silica by weight
- C03C3/064—Glass compositions containing silica with less than 40% silica by weight containing boron
- C03C3/066—Glass compositions containing silica with less than 40% silica by weight containing boron containing zinc
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/04—Glass compositions containing silica
- C03C3/076—Glass compositions containing silica with 40% to 90% silica, by weight
- C03C3/089—Glass compositions containing silica with 40% to 90% silica, by weight containing boron
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/12—Silica-free oxide glass compositions
- C03C3/14—Silica-free oxide glass compositions containing boron
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/12—Silica-free oxide glass compositions
- C03C3/14—Silica-free oxide glass compositions containing boron
- C03C3/145—Silica-free oxide glass compositions containing boron containing aluminium or beryllium
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/12—Silica-free oxide glass compositions
- C03C3/14—Silica-free oxide glass compositions containing boron
- C03C3/15—Silica-free oxide glass compositions containing boron containing rare earths
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C3/00—Glass compositions
- C03C3/12—Silica-free oxide glass compositions
- C03C3/14—Silica-free oxide glass compositions containing boron
- C03C3/15—Silica-free oxide glass compositions containing boron containing rare earths
- C03C3/155—Silica-free oxide glass compositions containing boron containing rare earths containing zirconium, titanium, tantalum or niobium
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C9/00—Emergency protection arrangements structurally associated with the reactor, e.g. safety valves provided with pressure equalisation devices
- G21C9/016—Core catchers
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C9/00—Emergency protection arrangements structurally associated with the reactor, e.g. safety valves provided with pressure equalisation devices
- G21C9/02—Means for effecting very rapid reduction of the reactivity factor under fault conditions, e.g. reactor fuse; Control elements having arrangements activated in an emergency
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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
- G21F1/00—Shielding characterised by the composition of the materials
- G21F1/02—Selection of uniform shielding materials
- G21F1/06—Ceramics; Glasses; Refractories
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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
- G21F9/28—Treating solids
- G21F9/30—Processing
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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
- G21F9/28—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
- G21F9/305—Glass or glass like matrix
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
Definitions
- the present invention relates to a neutron absorbing glass, a neutron absorbing material using the neutron absorbing glass, a molten fuel management method, a molten fuel take-out method and a reactor shutdown method using the neutron absorbing glass.
- a plurality of fuel assemblies including nuclear fuel material are loaded in the reactor core.
- nuclear fuel material uranium pellets
- the fuel assembly is designed to be of a size that is not critical as a whole, so there is a risk that it will become critical if the fuel assembly is unloaded one by one. And can be safely carried out.
- molten fuel molten nuclear fuel material
- This molten fuel is accumulated in the reactor pressure vessel or leaked into the containment vessel. Further, the molten fuel is obtained by melting uranium pellets in the fuel rods inside the nuclear reactor together with surrounding structures. In addition, it is necessary to cut the molten fuel and carry it out of the nuclear reactor. In such a case, a removal method for preventing the occurrence of criticality is indispensable.
- Patent Document 1 discloses SiO 2 , B 2 O 3 , Al 2 O 3 , La 2 O 3, Gd 2 O 3, and the like for transparent window glass having the ability to shield radiation such as X-rays and ⁇ -rays. Including glass compositions have been proposed. From Examples of Patent Document 1, SiO 2 is 18 to 30 mol%, B 2 O 3 is 18 to 38 mol%, Al 2 O 3 is 2.8 to 19.8 mol%, La 2 O 3 is 6 to 13 mol%, and Seven types of glass compositions with Gd 2 O 3 in the range of 15-20 mol% are specifically disclosed.
- B boron
- boric acid reacts with water to produce boric acid
- glass containing B if glass containing B is present in water, B may be dissolved from the glass to form boric acid and dissolve in water.
- boric acid dissolves in water, the inside of the furnace becomes an acidic corrosive environment, which may corrode the internal structure and peripheral equipment.
- the glass composition described in Patent Document 1 has improved detergent resistance and acid resistance so that no burns will occur even if it is washed.
- This glass composition contains a large amount of neutron absorption Gd (gadolinium) and B, so it can absorb neutrons, but the water resistance of the glass is low, and the problem that B dissolves when used for a long time in the state of being immersed in water. is there.
- the present invention aims to improve the water resistance of neutron absorbing glass.
- the present invention provides a neutron absorbing glass that can be put into water, containing gadolinium oxide, boron oxide and zinc oxide, and containing 42 to 65 mol% of B 2 O 3 in terms of the following oxides. It is characterized by that.
- the water resistance of the neutron absorbing glass can be improved.
- the B 4 C powder which is an example of a schematic external view of a neutron absorbing material sintered at neutron absorbing glass.
- the B 4 C particulate which is an example of a schematic cross-sectional view of a neutron absorbing material coated with a neutron absorbing glass. It is an example of the schematic sectional drawing of the state which the neutron absorber (neutron absorption glass or neutron absorption material) contacted the surface of the molten fuel. It is an example of the schematic sectional drawing of the method of taking out safely the molten fuel inside a nuclear reactor to the exterior of a nuclear reactor. It is a differential thermal analysis (DTA) curve of a typical glass. It is an example of the schematic sectional drawing of the installation which produces neutron absorption glass. It is an example of the schematic sectional drawing of the installation which produces a neutron absorption material.
- DTA differential thermal analysis
- the present invention relates to a neutron absorbing glass and a neutron absorbing material that are used in a reactor using water as a moderator, and is particularly suitable when used by being put into water in the reactor.
- the present invention also relates to a molten fuel management method, a molten fuel take-out method, and a reactor shutdown method to which the neutron absorbing glass or the neutron absorbing material is applied.
- the neutron absorbing glass of the present embodiment contains gadolinium oxide, boron oxide and zinc oxide, and B 2 O 3 is 42 to 65 mol% in terms of the following oxides. can get.
- the improved water resistance makes it easier for B to absorb neutrons to dissolve in water, thus facilitating water treatment and disposal. Note that when the oxide is described as “x to y mol%” in the text, it indicates that “x mol% to y mol%” (x mol% ⁇ oxide ⁇ y mol%). The same applies to the following.
- Gd is expensive, it is an element having a neutron absorption cross section about 60 times that of B. By containing Gd in glass, neutron absorption can be increased. Gadolinium oxide and boron oxide are mainly responsible for neutron absorption. Table 1 shows elements with large neutron absorption and their neutron absorption cross sections. Although depending on the state of radiated neutrons, elements with a larger neutron absorption cross section tend to have higher neutron absorption performance.
- the B 2 O 3 content (42 to 65 mol%) has been greatly increased, but on the other hand, the water resistance is lowered, so that oxidation is effective in improving water resistance. Contains zinc. Moreover, glass manufacturability is also improved by containing zinc oxide. Furthermore, the total of Gd 2 O 3 , B 2 O 3 and ZnO in terms of the following oxides is 70 mol% or more, which is effective for achieving all of glass manufacturability, water resistance and neutron absorption performance. It is.
- the preferred composition range of the neutron absorbing glass is 5 to 13 mol% Gd 2 O 3 in terms of the following oxide, 42 to 65 mol% B 2 O 3 , 5 to 45 mol% ZnO, Al 2 O 3 ,
- the total of one or more of ZrO 2 and R 2 O (R: alkali metal) is 0 to 30 mol%.
- water resistance can be improved without promoting crystallization, that is, without reducing glass manufacturability.
- the content is too high, the viscosity at high temperature increases with Al 2 O 3 , and crystallization occurs with ZrO 2 , thereby reducing the glass productivity.
- R 2 O there is a possibility that problems such as a significant increase in the volatilization amount of B 2 O 3 and conversely a decrease in water resistance may occur.
- Gd 2 O 3 and B 2 O 3 is 52 to 70 mol% and the total of ZnO, Al 2 O 3 , ZrO 2 and R 2 O is 30 to 48 mol% in terms of the following oxides.
- Gd 2 O 3 is 5 to 10 mol%
- B 2 O 3 is 47 to 60 mol%
- ZnO is 10 to 40 mol%
- Al 2 O 3 is 0 to 20 mol%
- ZrO 2 is 0 to 15 mol%
- 0 to 15 mol% of R 2 O are particularly effective for all of neutron absorption performance, water resistance and glass manufacturability.
- R 2 O is preferably at least Li 2 O.
- Li is smaller than the neutron absorption cross sections of Gd and B as shown in Table 1, but is one of the elements with large neutron absorption. Therefore, by including Li 2 O in the neutron absorption glass, neutron absorption performance Can be improved.
- R 2 O when two or more types of R 2 O (for example, Li 2 O and Na 2 O, Li 2 O and K 2 O, etc.) are contained, a mixed alkali effect peculiar to glass can be expressed, and glass manufacturability and water resistance are improved. it can.
- R 2 O is added too much, attention must be paid because the volatilization amount of B is remarkably increased at the time of glass production, and the water resistance is decreased. Further, the inclusion of R 2 O can express an unusual phenomenon of boric acid unique to glass, and can suppress or prevent elution of B into water.
- the density of the neutron absorbing glass is 3.2 to 4.7 g / cm 3 , it is possible to settle stably even if it is put into water.
- suitable shape and size it does not fly underwater by the circulation of water, but can be deposited on molten fuel stably.
- the shape include (a) spherical, (b) tablet, (c) granular, or (d) bead-like neutron absorbing glass 1 as shown in FIG.
- glass is a material with good thermoformability, and thus the shapes (a) to (d) can be produced at low cost.
- an appropriate average size is less than 10 mm mesh and 1 mm mesh or more. If the size is too large, there is a possibility that the molten fuel will not catch on the molten fuel due to being caught in the middle or difficult to contact the molten fuel. On the other hand, if the size is too small, there is a possibility that the water will fly underwater. A more preferable average size is less than 7 mm mesh and 2 mm mesh or more.
- the neutron absorbing material of the present embodiment is a neutron absorbing material 3 obtained by sintering B 4 C (boron carbide) particles 2 containing a large number of B having high neutron absorption performance with neutron absorbing glass 1 ′ as shown in FIG. . Further, as shown in FIG. 3, a neutron absorbing material 3 ′ in which the surface of granular B 4 C2 ′ is covered with the neutron absorbing glass 1 ′.
- B 4 C is one of the commonly known neutron absorbing materials and is widely used in nuclear reactors as a neutron shielding material and a nuclear reaction control material. For example, in boiling water reactors, control rods packed with B 4 C are used to control nuclear fission reactions during normal operation and emergencies.
- B 4 C is difficult to sinter by itself, and B may elute into water due to surface oxidation or the like, which may create an acidic corrosive environment.
- B 4 C and the neutron absorption glass of the present embodiment it becomes easy to obtain a desired shape and size, and good water resistance and neutron absorption performance can be obtained.
- FIG. 4 shows that the neutron absorber 18 (neutron absorbing glass 1 or neutron absorbing material 3 or 3 ′) contacts the containment vessel accumulated in the reactor pressure vessel or the surface of the molten fuel 5 leaking into the containment vessel. Shows the state.
- the neutron absorber 18 is introduced into the underwater 4 from above the molten fuel 5 managed in the underwater 4.
- the neutron absorber 18 is in contact with the molten fuel 5 or is present in the vicinity of the molten fuel 5, the neutron from the molten fuel 5 can be absorbed and the subcritical state of the molten fuel 5 can be maintained.
- Fig. 5 shows a schematic cross-sectional view of a method for safely taking out the molten fuel in which the uranium pellets and the like in the fuel rod are dissolved together with the surrounding structures to the outside of the reactor.
- the molten fuel 5 is excavated from the state shown in FIG. 4 (the state where the neutron absorber 18 is in contact with the surface of the molten fuel 5). Molten fuel 5 'flies underwater due to excavation, but the neutron absorber 18 also flies along with the molten fuel 5' to prevent recriticality and safely take out the molten fuel 5 'outside the reactor. Can do.
- the excavator 8 having the suction pipe 7 around the drill 6 is used, the excavated molten fuel 5 ′ can be sucked while being cut, so the amount scattered around is reduced, and the outside of the reactor can be more safely removed. It is possible to take it out.
- the reactor shutdown method of the present embodiment is a method of shutting down the reactor in an emergency, and the neutron absorbing glass or neutron absorbing material of the present embodiment is introduced into the reactor, When the neutron absorbing glass or neutron absorbing material of the present embodiment is deposited around the fuel rod, it is possible to prevent reaching the criticality.
- the manufacturability of neutron absorbing glass was evaluated in the state of glass produced at 1300-1400 ° C.
- the glass was mixed and mixed with a predetermined amount of glass material 500 g in a crucible, and heated to 1300-1400 ° C. at a heating rate of about 10 ° C./min in an electric furnace to melt. At that time, the mixture was kept for 2 to 3 hours with stirring to make the glass uniform. Thereafter, the crucible was taken out from the electric furnace, and the melt therein was poured into a stainless steel jig that had been heated to about 250 ° C. in advance to produce glass.
- the water resistance of the neutron absorbing glass was judged by the state of the glass after the glass prepared in an aqueous solution having a salt concentration of 0.9% by weight was boiled for 3 hours.
- the introduced glass did not change in appearance and no corrosion was observed, it was evaluated as “good”, and when the surface of the glass was white burned or the glass was structurally broken, it was evaluated as “failed”.
- the pH of water after the test was also measured, and even if no change in appearance was observed, it was set as “ ⁇ ” if it was acidic.
- the density of the neutron absorbing glass was measured by pycnometer method using powdered glass and helium gas.
- FIG. 6 shows a DTA curve of a typical glass. Starting temperature transition point T g of the first endothermic peak, the peak temperature is yield point M g. These characteristic temperature is defined by the viscosity, T g 10 13.3 poise, M g is equivalent to a temperature at which the viscosity of 10 11 poise.
- the neutron absorption performance of the neutron absorption glass is determined by using the quantities of Gd element, B element and Li element per unit volume obtained from the composition and density of the glass, and the neutron absorption cross sections of each element shown in Table 1.
- the neutron absorption cross section per unit volume was calculated, and when the density was equal to or greater than B 4 C of 2.52 g / cm 3 , it was evaluated as “good”, and when it was lower, it was evaluated as “failed”.
- Example 1 the composition and characteristics of neutron absorbing glass were examined. Examples are shown in Table 2, and Comparative Examples are shown in Table 3.
- the glasses of Examples A-01 to 30 passed all of the neutron absorption performance, water resistance and glass manufacturability. Also, the density is in the range of 3.2 to 4.7 g / cm 3 , and it is possible to settle stably even when thrown into water.
- B 4 C has a density of 2.52 g / cm 3 , which is larger than that.
- T g and sag M g is a characteristic temperature, secondary processing is likely due to heat. Specifically, (a) the spherical shape shown in FIG. 1 can be heated and pressed (b) into a tablet shape, or the cullet can be heated (c) into a granular shape.
- Comparative Examples B-01 and B-02 were general borosilicate glass and zinc borate glass, and had good glass manufacturability and water resistance. However, since it does not contain a Gd element having a large neutron absorption, the neutron absorption cross-section ratio is remarkably small and inferior to the neutron absorption performance of B 4 C compared to Examples A-01 to 30. Further, the density of Comparative Example B-02 was higher than that of B 4 C, but the density of Comparative Example B-01 was lower than that of B 4 C.
- Comparative Example B-03 ⁇ 05 are Gd 2 O 3 -B 2 O 3 based glass or a Gd 2 O 3 -B 2 O 3 -SiO 2 based glass, glass manufacture was good, B 2 The O 3 content was very high and the water resistance was insufficient. Comparative Example B-06 is also a Gd 2 O 3 —B 2 O 3 —SiO 2 glass, but because of the high content of SiO 2 , the high-temperature viscosity was large and the glass productivity was not good. Further, the water resistance was not sufficient.
- Comparative examples B-07 to 18 are commonly known ZnO, Al 2 O 3 , and ZrO in order to improve the water resistance and glass manufacturability of Gd 2 O 3 —B 2 O 3 —SiO 2 glass. 2 and alkaline earth oxides. However, it became cloudy due to crystallization, and sufficient water resistance could not be obtained. Inclusion of ZnO, Al 2 O 3 , ZrO 2 or alkaline earth oxide in Gd 2 O 3 -B 2 O 3 -SiO 2 glass should not lead to improvement of glass manufacturability and water resistance. I understood.
- Comparative Examples B-19 to 25 the inclusion of alkali metal oxides was examined, but only Comparative Example B-19 containing no Al 2 O 3 , ZnO, ZrO 2 and alkaline earth oxides was uniformly transparent. In other cases, white turbidity due to crystallization occurred as in Comparative Examples B-07 to 18. However, since Comparative Example B-19 contained a large amount of alkali metal oxide, the volatilization amount of B 2 O 3 was large and the water resistance was insufficient. The water resistance of Comparative Examples B-20 to 25, which had become white turbid (crystallized), was not as good as Comparative Examples B-07 to 18.
- the neutron absorbing glass that can be put into water contains gadolinium oxide, boron oxide, and zinc oxide. It has been found that glass manufacturing properties, water resistance and neutron absorption performance can all be improved when B 2 O 3 is 42 to 65 mol%.
- Example 2 the shape and size of the neutron absorption glass were examined. Since glass has good moldability by heat, we made neutron-absorbing glasses of various shapes and sizes.
- the neutron absorbing glass of Example A-20 was melted at 1300 to 1400 ° C. in the glass melting furnace 11 and the stirring blade 12 was rotated to make the molten glass 13 uniform.
- the plunger 14 By raising the plunger 14 from the lower part of the glass melting furnace 11, a predetermined amount of the molten glass 13 is poured out, sequentially cut by the cutters 15 and 15 ', and dropped between the rotating forming rolls 16 and 16'. It was.
- semi-circular grooves are continuously formed on the surfaces of the forming rolls 16 and 16 ', and the grooves face each other.
- the molten glass 13 that passed between the forming rolls 16 and 16 ′ was cooled and turned into a spherical neutron absorbing glass 1. Then, to remove thermal strain of the neutron-absorbing glass 1 of the resulting spherical, it was performed stress relief at a temperature slightly higher than the transition point T g. Transition point T g of the Example A-20 is because it is 493 ° C., and stress relief heat treatment at about 500 ° C.. By removing the thermal strain, the mechanical strength and water resistance of the neutron absorbing glass can be improved.
- the average size of the spherical neutron-absorbing glass 1 is roughly determined by the flow rate of the molten glass 13 from the glass melting furnace 11, the cutting speed of the cutters 15 and 15 ', and the groove size of the surfaces of the forming rolls 16 and 16'. Can be controlled. In this example, the diameter was adjusted to about 5 mm. Then, using a 10 mm mesh and a 1 mm mesh sieve, a size of less than 10 mm mesh and 1 mm mesh or more was obtained. With such a size, a spherical neutron absorbing glass can be obtained with a high yield.
- the size is 10 mm or more, there is a possibility that the molten fuel may not be spread over the molten fuel due to being caught in the middle when it is poured into the water or difficult to contact the molten fuel.
- the size is less than 1 mm, there is a risk that the water will drift underwater.
- a 7 mm mesh and a 2 mm mesh sieve are used and the mesh is less than 7 mm and 2 mm mesh or more.
- a tablet-like neutron absorbing glass shown in FIG. 1 was produced using the glass of Example A-20 in the same manner as described above.
- the tablet-shaped neutron absorbing glass was produced by hot pressing the spherically produced neutron absorbing glass. Thereafter, in the same manner as described above, the strain was removed and sieved to obtain a desired size. Since the tablet shape is less likely to roll than the spherical shape, handling is easy. Further, since the surface area per weight is larger than that of a sphere, an improvement in neutron absorption performance can be expected.
- the (c) granular neutron absorbing glass shown in FIG. 1 was also produced using the glass of Example A-20 in the same manner as described above.
- the glass of Example A-20 was melted and produced, and pulverized to an appropriate size cullet by a crusher.
- the cullet was heated to about 750 ° C. in a tunnel furnace, and the edges were rounded to form particles. At that time, the same tunnel furnace was also used for strain relief. Thereafter, a sieve was applied in the same manner as described above to obtain a desired size.
- the (d) bead-like neutron absorbing glass shown in FIG. 1 was also produced using the glass of Example A-20 in the same manner as described above.
- a glass tube having a diameter of about 5 mm was produced from the glass of Example A-20.
- the glass tube was scratched at intervals of about 5 mm and cut by thermal shock. This was heated to about 750 ° C. in a tunnel furnace in the same manner as described above, and the edges were rounded to form beads. At that time, the same tunnel furnace was also used for strain relief. Thereafter, a sieve was applied in the same manner as described above to obtain a desired size. In the bead shape, the surface area can be further increased, which is considered to contribute to the improvement of neutron absorption performance.
- Example 3 the combination of neutron absorption glass and B 4 C was studied.
- Neutron-absorbing glass and B 4 C powder were mixed, molded in a mold, and heated in a low-oxygen atmosphere to produce the sintered neutron-absorbing material shown in FIG.
- the reason for heating in a low oxygen atmosphere is to suppress or prevent the oxidation of B 4 C as much as possible.
- the neutron absorbing glass the glass of Example A-14 shown in Table 2 was used and pulverized to 30 ⁇ m or less by a stamp mill and a jet mill.
- B 4 C used a commercially available powder of 150 ⁇ m or less.
- the neutron-absorbing glass powder of Example A-14 was mixed and mixed at a ratio of 25% by volume and B 4 C powder at a rate of 75% by volume, and the diameter was 5 mm and the thickness was 5 mm under the condition of 1 ton / cm 2 using a mold. A large number of cylindrical shaped bodies were produced. These compacts were passed through a tunnel furnace in a low-oxygen atmosphere, and the glass powder of Example A-14 was softened and fluidized at about 800 ° C. to produce a sintered body of a neutron absorbing material. The obtained sintered body had a volume shrinkage of about 10 to 20%.
- Example 1 As a result of carrying out the same water resistance test as in Example 1 using the obtained sintered body, good water resistance was obtained without being corroded. Moreover, since both the glass of Example A-14 and B 4 C have a large neutron absorption cross section per unit volume, the neutron absorption performance is good. On the other hand, B 4 C alone may react with water gradually in water to produce boric acid, resulting in an acidic corrosive environment. By combining with neutron absorbing glass, the area where B 4 C comes into contact with water can be reduced, and the water resistance of neutron absorbing glass is high, so that B does not easily dissolve even when exposed to water for a long time. Moreover, it becomes easy to make a sintered body of B 4 C.
- this neutron absorbing material is not limited to the application to be put into water, but can be developed for substitution of B 4 C powder loaded in a control rod, substitution of a B 4 C sintered body used in a fast reactor, and the like.
- Example 4 in the same manner as in Example 3, the combination of neutron absorbing glass and B 4 C was studied, and the neutron absorbing material 3 ′ shown in FIG. 3 was produced.
- the neutron absorbing glass 1 ′ the glass of Example A-25 shown in Table 2 was used.
- the B 4 C particles 2 ′ commercially available granular particles of 1 to 3 mm were used.
- FIG. 8 shows the equipment used for producing the neutron absorbing material 3 ′ shown in FIG. In FIG. 8, the equipment shown in FIG. 7 is devised so that granular B 4 C particles 2 ′ can be introduced from the plunger 14 into the molten glass 13 at 1300 to 1400 ° C.
- the B 4 C particles 2 ′ were introduced into the upper container 17 of the glass melting furnace 13 and heated with the residual heat of the glass melting furnace 13. Further, in order to prevent oxidation of B 4 C, the inside of the container 17 was made an inert atmosphere. Granular B 4 C particles 2 ′ were sequentially dropped from the container 17, and were poured from the lower part of the glass melting furnace 11 together with the molten glass 13. It was cut with cutters 15 and 15 ′ and dropped between forming rolls 16 and 16 ′ in the same manner as in Example 2 to produce a spherical neutron absorbing material 3 ′ as shown in FIG.
- neutron absorption glass is applied to the surface portion of one B 4 C particle.
- Example 4 there were many cases where a plurality of B 4 C particles entered. This is not a problem unless the size of the neutron absorbing material 3 ′ becomes too large. Thereafter, the resulting neutron absorbing material 3 'was subjected to heat treatment slightly temperatures greater about 510 ° C. above the transition point T g of the Example A-25, the neutron absorbing glass 2' to remove heat distortion.
- Example 1 The same water resistance test as that of Example 1 was performed using the obtained neutron absorbing material. As a result, good water resistance was obtained without being corroded. Further, regarding the neutron absorption performance, it goes without saying that both the glass of Example A-25 and B 4 C have a large neutron absorption cross-sectional area per unit volume, and thus are good.
- the fourth embodiment as compared to Example 3, and the neutron absorbing glass powder, B 4 C powder and uniformly mixed, molded, does not require firing, the neutron absorbing glass and B 4 C The neutron absorbing material can be manufactured at low cost.
- this neutron absorbing material is not limited to the application to be put into water, but it is an alternative to the B 4 C powder loaded in the control rod or the B 4 C sintered body used in the fast reactor. There is a possibility that it can also be deployed.
- Example 5 an example of a molten fuel management method to which the neutron absorbing glass or neutron absorbing material of the present invention examined in Examples 1 to 4 is applied will be described.
- Neutron-absorbing glass or neutron-absorbing material is introduced into the reactor to maintain the subcriticality of the molten fuel and enhance safety.
- a lump of molten fuel 5 is submerged in water 4, and a neutron absorber 18 (neutron absorbing glass, neutron absorbing material) is introduced into water 4 so as to directly cover the upper surface of the lump of molten fuel 5. Touching. Since the density of the neutron absorber 18 is sufficiently larger than that of water, it is likely to deposit on the surface of the molten fuel 5. Further, when there are cracks in the molten fuel 5 mass or when there is a gap between the molten fuel 5 masses, the neutron absorber 18 enters these cracks or gaps.
- the neutrons generated from the molten fuel 5 are shielded and the chain reaction is suppressed so that the criticality is not reached. can do. It is effective to make the size of the neutron absorber 18 smaller than the mass of the molten fuel 5.
- the neutron absorbing glass is a uniform transparent glass, but has a characteristic of being colored by neutron irradiation. Since the degree of coloring tends to increase as the amount of neutron irradiation increases, the position of the molten fuel in the nuclear reactor is detected by examining the degree of coloring of the neutron absorbing glass of the present invention introduced into the nuclear reactor. It is also possible to make predictions.
- the neutron absorber 18 is introduced into the reactor so as not to cause recriticality when the molten fuel 5 is taken out.
- the molten fuel 5 is crushed by the drill 6 of the excavator 8 and the particulate molten fuel 5 ′ is sucked through the suction pipe 7 of the excavator 8.
- a part of the excavated particulate molten fuel 5 ′ may not be sucked into the suction pipe 7 of the excavator 8 and may be scattered in the surrounding water 4.
- the volume ratio of the particulate molten fuel 5 ′ in the water 4 changes and becomes recritical.
- the neutron absorber 18 is also scattered together with the particulate molten fuel 5 ′ scattered in the water 4 so that neutrons in the water 4 can be absorbed and blocked. Thereby, a chain reaction can be suppressed and it can prevent reaching a recriticality also during excavation work. Further, even if the neutron absorber 18 is damaged by cutting with the drill 6 of the excavator 8 during excavation work, the neutron absorption performance is not impaired.
- the excavating method may be a power shovel and is not limited to an excavator.
- Example 7 describes an example of controlling a nuclear fission reaction by introducing neutron absorbing glass or neutron absorbing material.
- the above-mentioned neutron absorbing glass or neutron absorbing material is introduced so that the neutron absorbing glass or neutron absorbing material is deposited around the fuel rod inside the reactor.
- the nuclear fission reaction of the nuclear reactor can be controlled and the nuclear reactor can be stopped urgently.
- neutron absorbing glass or neutron absorbing material it is possible to prevent boric acid from eluting into the water inside the reactor, or to prevent pH from being lowered even if boric acid is eluted. For this reason, corrosion of the reactor internal structure can be prevented and the reaction of the nuclear fuel can be continuously suppressed, so that the nuclear reactor can be stopped for a long period of time.
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Abstract
Description
このガラス管を長さ5mm程度の間隔で傷を付け、熱衝撃でカットした。これを、上記同様にトンネル炉で約750℃にまで加熱して、エッジ部を丸めることによって、ビーズ状とした。その際に同じトンネル炉で歪取りも同時に行った。その後、上記と同様にふるいをかけ、所望のサイズを得た。ビーズ状では、さらに表面積を大きくできることから、中性子吸収性能の向上に貢献できるものと考えられる。
2, 2’:B4C粒子
3, 3’:中性子吸収材料
4:水中
5, 5’:溶融燃料
6:ドリル
7:吸引管
8:切削機
11:ガラス溶融炉
12:撹拌羽
13:溶融ガラス
14:プランジャー
15, 15’:カッター
16, 16’:成形ロール
17:容器
18:中性子吸収体
Claims (15)
- 水中に投入可能な中性子吸収ガラスにおいて、酸化ガドリニウム、酸化ホウ素及び酸化亜鉛を含み、次の酸化物換算でB2O3を42~65モル%含むことを特徴とする中性子吸収ガラス。
- 請求項1において、次の酸化物換算でGd2O3、B2O3及びZnOの合計が70モル%以上であることを特徴とする中性子吸収ガラス。
- 請求項1又は2において、次の酸化物換算でGd2O3を5~13モル%、B2O3を42~65モル%、ZnOを5~45モル%含み、Al2O3、ZrO2及びR2O(R:アルカリ金属)のうち1種以上を合計0~30モル%含むことを特徴とする中性子吸収ガラス。
- 請求項1乃至3の何れかにおいて、次の酸化物換算でGd2O3とB2O3の合計が52~70モル%、ZnO、Al2O3、ZrO2及びR2Oの合計が30~48モル%であることを特徴とする中性子吸収ガラス。
- 請求項1乃至4の何れかにおいて、次の酸化物換算でGd2O3を5~10モル%、B2O3を47~60モル%、ZnOを10~40モル%、Al2O3を0~20モル%、ZrO2及0~15モル%及びR2Oを0~15モル%含むことを特徴とする中性子吸収ガラス。
- 請求項3乃至5の何れかにおいて、前記R2Oが少なくともLi2Oを含むことを特徴とする中性子吸収ガラス。
- 請求項1乃至6の何れかにおいて、前記中性子吸収ガラスの密度が3.2~4.7g/cm3であることを特徴とする中性子吸収ガラス。
- 請求項1乃至7の何れかにおいて、前記中性子吸収ガラスの形状が粒状、球状、タブレット状或いはビーズ状であることを特徴とする中性子吸収ガラス。
- 請求項1乃至8の何れかにおいて、前記中性子吸収ガラスの平均サイズが10mmメッシュ未満1mmメッシュ以上であることを特徴とする中性子吸収ガラス。
- B4C粉末と請求項1乃至9の何れかの中性子吸収ガラスとを含むことを特徴とする中性子吸収材料。
- 粒状のB4Cの表面に請求項1乃至9の何れかの中性子吸収ガラスが被覆されたことを特徴とする中性子吸収材料。
- 原子炉圧力容器内又は格納容器内の溶融燃料の管理方法において、請求項1乃至8の何れかの中性子吸収ガラス、又は請求項10若しくは11の中性子吸収材料を水中に配置された前記溶融燃料に向けて投入し、前記中性子吸収ガラス又は前記中性子吸収材料を前記溶融燃料の表面に接触させることを特徴とする溶融燃料の管理方法。
- 原子炉の内部の溶融燃料を前記原子炉の外部に取り出す方法において、請求項1乃至8の何れかの中性子吸収ガラス、又は請求項10若しくは11の中性子吸収材料を水中に配置された前記溶融燃料に向けて投入し、前記中性子吸収ガラス又は前記中性子吸収材料が前記溶融燃料の表面に接触させ、前記溶融燃料を砕いて前記原子炉の外部に取り出すことを特徴とする溶融燃料の取り出し方法。
- 請求項13において、前記溶融燃料を砕きながら吸引することにより、前記原子炉の外
- 原子炉の停止方法において、前記原子炉の内部に請求項1乃至9の何れかの中性子吸収ガラス、又は請求項10若しくは11の中性子吸収材料を投入し、前記中性子吸収ガラス又は前記中性子吸収材料が前記原子炉の内部の燃料棒の周囲に堆積させることを特徴とする原子炉の停止方法。
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PCT/JP2013/069578 WO2015008370A1 (ja) | 2013-07-19 | 2013-07-19 | 中性子吸収ガラス及びそれを用いた中性子吸収材料、並びにこれらを適用した溶融燃料の管理方法、溶融燃料の取り出し方法及び原子炉の停止方法 |
JP2015527118A JP6038323B2 (ja) | 2013-07-19 | 2013-07-19 | 中性子吸収ガラス及びそれを用いた中性子吸収材料、並びにこれらを適用した溶融燃料の管理方法、溶融燃料の取り出し方法及び原子炉の停止方法 |
US14/904,211 US20160155521A1 (en) | 2013-07-19 | 2013-07-19 | Neutron-absorbing glass and neutron-absorbing material using the same, and management method of corium, unloading method of corium, and shutdown method of nuclear reactor to which the same is applied |
TW103119017A TWI547463B (zh) | 2013-07-19 | 2014-05-30 | Neutron absorbing glass and the use of the neutron absorbing material thereof, and the management method of the fused fuel to which they are applied, the method of removing the molten fuel and the stopping method of the atomic furnace |
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PCT/JP2013/069578 WO2015008370A1 (ja) | 2013-07-19 | 2013-07-19 | 中性子吸収ガラス及びそれを用いた中性子吸収材料、並びにこれらを適用した溶融燃料の管理方法、溶融燃料の取り出し方法及び原子炉の停止方法 |
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JP6452780B1 (ja) * | 2017-10-12 | 2019-01-16 | 一般社団法人Nb研究所 | 燃料デブリの回収方法 |
JP2020056800A (ja) * | 2020-01-08 | 2020-04-09 | 国立研究開発法人 海上・港湾・航空技術研究所 | 溶融核燃料収納容器用の粒状体の製造方法、及び溶融核燃料収納容器 |
JP2020125905A (ja) * | 2019-02-01 | 2020-08-20 | 一般社団法人Nb研究所 | 燃料デブリの処理方法 |
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US11309096B1 (en) * | 2018-07-25 | 2022-04-19 | National Technology & Engineering Solutions Of Sandia, Llc | Injectable sacrificial material systems and methods to contain molten corium in nuclear accidents |
CN115368011B (zh) * | 2022-09-09 | 2023-06-23 | 中国建筑材料科学研究总院有限公司 | 用于光纤传像元件的相容性匹配良好的芯皮玻璃及其制备方法 |
CN115611513B (zh) * | 2022-10-28 | 2024-06-04 | 南京玻璃纤维研究设计院有限公司 | 一种耐辐射玻璃材料及其制备方法与应用 |
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JP2020056800A (ja) * | 2020-01-08 | 2020-04-09 | 国立研究開発法人 海上・港湾・航空技術研究所 | 溶融核燃料収納容器用の粒状体の製造方法、及び溶融核燃料収納容器 |
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JP6038323B2 (ja) | 2016-12-07 |
JPWO2015008370A1 (ja) | 2017-03-02 |
US20160155521A1 (en) | 2016-06-02 |
TW201505995A (zh) | 2015-02-16 |
TWI547463B (zh) | 2016-09-01 |
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