JP2011021923A - Method for measuring neutron irradiation amount and method for detecting nuclear fuel failure - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To achieve a method and device capable of easily determining a neutron irradiation amount which causes damage to a member used in a nuclear reactor. <P>SOLUTION: The method for measuring a neutron irradiation amount focuses on the fact that the composition (isotope ratio) of tagging gas (Xe, Kr) is changed in accordance with the neutron irradiation amount, and identifies a damaged detection target member and determines the neutron irradiation amount which causes the damage by making the detection target member include tagging gas having a predetermined composition; measuring the composition of the tagging gas released by damage of the detection target member; and calculating the changed amount of the composition. <P>COPYRIGHT: (C)2011,JPO&INPIT

Description

  The present invention relates to a neutron irradiation measurement method, a nuclear fuel damage detection method, and an apparatus for carrying out these methods.

  The tagging method, which is a method for detecting damaged fuel in fast reactors, is pre-clad with a labeling gas (tag gas) such as Xe (xenon) or Kr (krypton) with different isotope ratios for each fuel assembly (fuel rod). This is a technique for identifying a fuel rod that has been broken and released a tag gas by analyzing the isotope ratio of the tag gas that is sealed in a tube and released when the fuel is broken and moves to the cover gas space.

  This method is also applied to the identification of fractured specimens in an irradiation test in which a specimen is creep ruptured in a furnace. However, the neutron irradiation dose, which is an important parameter in the irradiation test, is determined by the multiple activation foil method. Separately measured and evaluated.

JP 2005-43133 A

  In the conventional irradiation test, the multiple activation foil method for measuring the neutron irradiation amount requires irradiation with several dosimeter sets according to the irradiation position of the test piece. After the irradiation test is completed, the irradiation test apparatus is taken out of the furnace and collected, and radiation measurement is performed. Also, due to the saturation and decay problems of the activation foil, the experimental value obtained is the average flux just before the end of irradiation, and the irradiation amount at the time of rupture of each specimen is separately calculated by integral calculation based on the operation history There is a hassle that must be done.

  One object of the present invention is to provide a method for measuring a neutron irradiation amount that can easily determine the amount of neutron irradiation that leads to breakage of a member used in a nuclear reactor.

  Another object of the present invention is to provide a nuclear fuel failure detection method capable of easily identifying a fuel rod damaged in a nuclear reactor. In particular, the type of tag gas set for the fuel rods mounted in the furnace can be reduced.

  Another object of the present invention is to provide a measurement device and a detection device suitable for realizing a neutron irradiation measurement method and a nuclear fuel damage detection method.

  Another object of the present invention is to provide an analysis device suitable for use in the measurement device and the detection device.

  The neutron irradiation measurement method of the present invention focuses on the fact that the composition (isotope ratio) of the tag gas (Xe, Kr) changes according to the neutron irradiation amount, and includes a tag gas having a predetermined composition in the detected member. In addition, by measuring the composition of the tag gas released when the detected member is damaged, and calculating the amount of change in the composition, the detected member is damaged and the amount of neutron irradiation resulting in the damage is obtained. .

  If the member to be detected is a material development test piece for nuclear reactor equipment, each test piece contains a tag gas having a different specific composition, and these test pieces are placed in the test reactor. Irradiation is performed, the composition of the tag gas released when the test piece is damaged is measured, and the amount of change in the composition is calculated, whereby the damaged test piece is identified and the neutron irradiation amount of the test piece is obtained.

  The nuclear fuel damage detection method for identifying fuel rods damaged in the nuclear reactor of the present invention pays attention to the fact that fuel exchange is performed at different times for each group, and the fuel rods installed in the nuclear reactor are those of the same replacement time. The tag gas is divided into a plurality of groups as one group, and the tag gas sealed in the fuel rod (in the fuel cladding tube) in each group is identified by measuring its composition when the fuel rod is broken and discharged. It is changed so that the identification within the group can be performed, and the fuel rod in each group is identified by the composition of the tag gas released when the fuel rod is broken. The amount of neutron irradiation from when the fuel rod is mounted is determined by calculating the amount of change in the composition of the fuel, and the mounting time (replacement time) is determined based on the amount of neutron irradiation.

  A measurement apparatus and a detection apparatus suitable for realizing the neutron irradiation measurement method and the nuclear fuel damage detection method of the present invention measure the composition of the tag gas released by the damage of the detected member, and the amount of change in the composition (isotope ratio). The amount of neutron irradiation can be determined based on the calculated amount of change in composition.

  An apparatus suitable for measuring the composition of the tag gas in such a measurement method and detection method irradiates a laser beam having a wavelength equal to the resonance energy specific to the element to be measured, and performs mass spectrometry by resonance excitation / ionization. This is a laser resonance ionization mass spectrometer, specifically, a resonance gas is excited and ionized by irradiating a sampling gas introduced into the ionization chamber with laser light, and the control electrode group passes the mass gate in the form of an ion beam. A gas ion beam is used, and the tag gas ion beam is reflected by a group of reflecting electrodes so that the tag gas ions (atoms / molecules) reach the microchannel plate in ascending order of mass and are converted into mass spectrum signals.

  The neutron irradiation measuring method of the present invention measures the composition of the tag gas released when the member to be detected is damaged, and calculates the amount of change, thereby damaging the member to be detected and the amount of neutron irradiation leading to the damage. Therefore, it is possible to easily determine the amount of neutron irradiation that leads to breakage of members used in the nuclear reactor.

  In the nuclear fuel damage detection method of the present invention, the tag gas sealed in the fuel rod (in the fuel cladding tube) is identified within each group by measuring the composition of the tag gas when the fuel rod is broken and released, and which group It is easy to identify the fuel rods by measuring the composition of the released tag gas and calculating the amount of change. Can be identified.

  The measuring device and the detecting device for realizing the neutron irradiation measuring method and the nuclear fuel damage detecting method of the present invention measure the composition of the tag gas released by the damage of the detected member, and the change amount of the composition (isotope ratio). The amount of change in the amount of neutron irradiation until the breakage is identified based on the composition of the released tag gas and the change in the composition. it can.

  The analyzer according to the present invention is configured to resonantly excite and ionize the introduced sampling gas by irradiating a laser beam, and to pass through a mass gate as an ion beam form by a control electrode group to form a tag gas ion beam. This tag gas ion beam The tag gas ions (atoms / molecules) reach the microchannel plate in ascending order of mass and are converted into mass spectrum signals by reflecting the light from the reflective electrode group, and released due to damage to the detected member. It is possible to accurately measure the composition of the tag gas and the composition according to the neutron irradiation amount, and to accurately determine the amount of change (isotope ratio).

It is a systematic diagram of the neutron irradiation amount measuring system of the present invention. It is a graph which shows the isotope ratio of Xe gas used as tag gas together with the neutron capture area. It is a characteristic view which shows the relationship between the neutron irradiation amount of Xe, and a composition change. It is a schematic diagram which shows the specific structure of a tag gas measuring device. It is a characteristic view which shows the mass spectrum obtained by measuring the isotope composition ratio of Xe tag gas by laser resonance ionization mass spectrometry.

The present invention pays attention to the fact that the composition (isotope ratio) of the tag gas changes according to the neutron irradiation amount, and the detected member is damaged by including the tag gas having a predetermined known composition in the detected member. Measure the composition of the tag gas released by the, calculate the amount of change in the composition, to determine the amount of neutron irradiation that leads to damage of the detected member,
When detecting breakage of a plurality of detected members and the amount of neutron irradiation, tag materials having different specific compositions are included in each detected member, and these detected members are placed in a test furnace and irradiated with radiation. By measuring the composition of the tag gas released when the detected member is damaged and calculating the amount of change in the composition, the identification of the damaged detected member and the neutron irradiation amount of the detected member are obtained. .

The amount of change in the composition of the tag gas is determined by calculating the change in the ratio of two predetermined isotopes. When Xe is used as a tag gas, it is preferable that the amount of change in the isotope ratio ( ¹³⁰ Xe / ¹²⁹ Xe) between ¹²⁹ Xe and ¹³⁰ Xe is obtained.

  The specific composition of the tag gas contained in each detected member when detecting the breakage of a plurality of detected members and the amount of neutron irradiation is the composition of the tag gas contained in the other detected member due to the change in composition caused by radiation irradiation. It is necessary to make them different from each other so that it is possible to avoid the identification of the member to be detected that has been confused and damaged and the inability to determine the neutron irradiation amount.

  The tag gas used to identify damaged parts to be detected and to detect the neutron irradiation amount of the detected member includes Xe and Kr, but has a large neutron reaction cross-section and measures a significant composition change. Xe is suitable as a gas that can be used, and it is desirable to use Xe in order to detect the neutron irradiation with high accuracy.

  FIG. 1 is a system diagram of a neutron irradiation measurement system. In this neutron irradiation measuring system, a creep rupture test piece 1 as a member to be detected is formed in a hollow shape, and helium gas (He) and a tag gas (Xe) having a predetermined (known) composition are mixed therein. Enclose and pressurize. The creep rupture test piece 1 configured as described above is installed in the core 3 a of the reactor vessel 3 by the irradiation device 2. A coolant 4 is circulated in the reactor vessel 3 and the upper space 5 is filled with a cover gas (Ar). The gas pipe 6 that opens into the upper space 5 of the reactor vessel 3 communicates the cover gas to the gas sampling device 7 and guides the cover gas to the gas sampling device 7. The tag gas measuring device 8 is configured to measure the composition of the tag gas contained in the cover gas periodically sampled by the gas sampling device 7. The computer 9 retains the initial composition data of the tag gas (Xe) sealed in the creep rupture test piece 1, acquires the measurement data from the tag gas measurement device 8, and compares the initial composition data with the measurement data to detect the detected tag gas. The composition (type) is identified and the amount of change in the composition is calculated to determine the neutron irradiation amount.

  The void detection device 10 is connected to a void detection thermocouple built in the irradiation device 2, and a detection signal of the void detection thermocouple (responds to a temperature fluctuation generated when the creep rupture test piece 1 is broken). The creep rupture test piece 1 is configured to detect that a rupture has occurred.

  In the neutron irradiation measuring system configured as described above, when the creep rupture test piece 1 installed in the core portion 3a of the reactor vessel 3 is broken by the irradiation device 2, it is output from the void detection thermocouple in the void detection device 10. Since the detection signal fluctuates, the rupture of the creep rupture test piece 1 can be detected. Then, the helium gas and the tag gas released from the creep rupture test piece 1 due to the breakage become bubbles 11 and rise in the coolant 4 and enter the cover gas in the upper space 5.

  The gas sampling device 7 periodically samples the cover gas and transfers it to the tag gas measuring device 8. The tag gas measuring device 8 measures the composition of the tag gas contained in the cover gas by mass analyzing the transferred cover gas by laser resonance ionization mass spectrometry.

  In the computer 9, the initial composition data of the tag gas (Xe) to be sealed in the creep rupture test piece 1 is input and held in advance, and the measurement data is acquired from the tag gas measuring device 8 and compared with the initial composition data. Identifies the gas of the initial composition data that approximates the composition shifted by the expected composition variation from the measured tag gas composition as the encapsulated tag gas and calculates the variation in the measured tag gas composition (isotope ratio) Find the neutron dose.

When a plurality of creep rupture test pieces 1 having different physical properties are subjected to a creep rupture test at the same time, the tag gas to be sealed has a unique composition (isotope ratio) that is different for each creep rupture test piece 1.
A tag gas (ruptured creep rupture test piece 1) encapsulating a gas having an initial composition data that approximates a composition shifted by the expected composition change amount from the measured tag gas composition by comparing the measured data with the initial composition data. At the same time, the amount of change in composition (isotope ratio) is calculated and the neutron irradiation amount is obtained.

  The relationship between the amount of neutron irradiation and the amount of change in the composition (isotope ratio) of the tag gas is obtained by preliminarily obtaining a table by measuring and calculating by the irradiation test for each type of tag gas to be sealed, In the fracture test, the amount of neutron irradiation is obtained by referring to a table based on the obtained composition (type) of tag gas and the amount of composition change.

  The gas sampling device 7 detachably provides a gas storage container for storing the sampled gas, and transports and connects the gas storage container to the tag gas measurement device 8 located far away from the gas sampling device 7 to thereby configure the composition of the tag gas. It is also possible to configure to measure. Such a configuration makes it possible to share the tag gas measurement device 8 as a gas measurement device of another system.

FIG. 2 is a graph showing the isotope ratio of the Xe gas used as the tag gas together with the neutron capture area. The isotope ratio is almost the same as the natural ratio. As the change in isotope ratio due to neutron irradiation, the cross-sectional area of ¹²⁴ Xe is the largest, but since the abundance ratio is small, the absolute value of the amount of change is small and the largest is ¹²⁹ Xe (n, γ) And ¹³⁰ Xe. Since the abundance ratio of the destination ¹³⁰ Xe is about 1/7 of the ^{129 Xe,} that determine the amount of change in the ratio of ¹²⁹ Xe and ^{130 Xe (130 Xe / 129 Xe} ) is best.

FIG. 3 shows the characteristics of Xe neutron irradiation and composition change. The isotope ratio ¹³⁰ Xe / ¹²⁹ Xe increases by 20% at a total neutron dose of 6.9 × 10 ²² n / cm ² . In the measurement of the tag gas released due to the breakage of the detected member, it is necessary to measure in advance Xe contained in the cover gas before release and subtract it from the measured value after release.

  FIG. 4 is a schematic diagram showing a specific configuration of the tag gas measuring device 8. The tag gas measuring device 8 is a device that measures the composition of the tag gas by laser resonance ionization mass spectrometry. The tag gas measuring device 8 irradiates a laser beam having a wavelength equal to the resonance energy specific to the element to be measured, and performs resonance excitation / ionization to obtain a mass. It is to be analyzed and, in principle, background ions are not generated, and the S / N ratio can be greatly improved. By configuring a very small amount of rare gas isotope analysis system using a tunable system and a time-of-flight mass spectrometer, the quantification limit ( The background fluctuation of 10σ) makes it possible to achieve 2 ppt for the Xe isotope and 5 ppt for the Kr isotope.

  The time-of-flight mass spectrometer 81 includes a sample gas ionization chamber portion 811 and a mass spectrometer tube portion 812.

  The sample gas ionization chamber 811 is highly evacuated by a turbo molecular pump 813 and a scroll pump 814, and a sampling gas is introduced into the ionization chamber from the gas sampling device 7 through a supersonic pulse molecular beam valve 8111. Resonance excitation and ionization are performed by irradiating the laser beam, and the control electrode group 8112 sends the ion beam 82 into the mass analysis tube unit 812. Laser light is introduced into the ionization chamber from a laser light entrance window 8113 and is led out from a laser light exit window 8114 with a polarizing filter.

  The mass analysis tube unit 812 is highly evacuated by the turbo molecular pump 815 and the scroll pump 816, and the ion beam 82 sent from the sample gas ionization chamber unit 811 is deflected by the mass gate 8121 to pass only the tag gas composition component. . The tag gas ion beam 82 that has passed through the mass gate 8121 is reflected by the reflective electrode group 8122 and is incident on the microchannel plate 8123 that is an ion detector. The tag gas ion beam (atom / molecule) 82 reaches the microchannel plate 8123 in ascending order of mass and is converted into a mass spectrum signal.

  The laser that irradiates the sampling gas introduced into the ionization chamber of the sample gas ionization chamber 811 uses a wavelength variable system 818 to resonate laser light oscillated by a YAG laser oscillator 817 using YAG for excitation at a wavelength suitable for sample gas ionization. The ion beam is adjusted to an ionization laser beam 83 and is narrowed by a lens 819 so as to be focused on a gas ionization unit, and is incident on the ionization chamber through a laser beam entrance window 8113.

The digital signal processing device 84 is linked with the computer 9 to control the supersonic pulse molecular beam valve 8111 and the YAG laser oscillator 817 and output from the microchannel plate 8123. As described above, the computer 9 is input in advance. The initial composition data of the tag gas (Xe), the composition change amount due to neutron irradiation (predicted value), and the neutron irradiation table indicating the relationship between the neutron irradiation amount and the change amount of the tag gas composition (isotope ratio) are held. In addition, by obtaining the measurement data from the tag gas measuring device 8 and comparing it with the initial composition data, the gas of the initial composition data that approximates the composition shifted by the expected composition change amount from the measured tag gas composition was sealed. Identify the tag gas and calculate the amount of change in composition (isotope ratio) and refer to the neutron irradiation table The process which calculates | requires the amount of neutron irradiation is performed.

Incidentally, FIG. 5 shows that a plurality of detected members filled with Xe tag gases having different compositions are subjected to a creep test in the furnace and irradiated with neutrons, and after the detected member breaks, the tag gas (test furnace cover gas) is collected and laser The mass spectrum obtained by measuring the isotopic composition ratio of the Xe tag gas by resonance ionization mass spectrometry is shown. The tag gas is diluted to a radionuclide concentration of 10 ⁰ to 10 ² ppb in the cover gas space, but a good mass spectrum is obtained by laser resonance ionization mass spectrometry, and the tag gas The composition (the fractured member to be detected) is identified, and the neutron irradiation amount can be obtained based on the amount of change in the isotope composition.

  When identifying broken fuel rods in a nuclear reactor, the fuel rods installed in the nuclear reactor are divided into multiple groups with the same replacement period as one group, and the fuel rods in each group (in the fuel cladding tube) The tag gas to be enclosed in () is changed so that identification can be performed within each group by measuring and identifying the composition when the fuel rod is broken and released. By using the tag gas measuring device 8 in the measured neutron irradiation measurement system, the cover gas in the reactor sampled periodically is measured, so that in each group based on the composition of the tag gas released when the fuel rod is broken The fuel rods are identified, and the group of fuel rods is identified by calculating the amount of change in the composition of the released tag gas to obtain the neutron irradiation amount from when the fuel rod was mounted. In Carried out in search of Zui and implementation time (time to replace).

  Since the neutron irradiation amount (exposure amount) of the fuel rod in the reactor can be calculated by the reactor operation time after the fuel rod is mounted, the relationship between the reactor operation time and the neutron irradiation amount (exposure amount) Is calculated and tabulated in advance and is stored in the computer 9 as an operation time table, and the operation time table is referred to by the neutron irradiation amount (exposure amount) obtained from the tag gas measurement result. Group).

  DESCRIPTION OF SYMBOLS 1 ... Creep rupture test piece, 2 ... Irradiation device, 3 ... Reactor vessel, 3a ... Core part, 4 ... Coolant, 5 ... Upper space, 6 ... Gas pipe, 7 ... Gas sampling device, 8 ... Tag gas measuring device, 9 DESCRIPTION OF SYMBOLS ... Computer, 11 ... Bubble, 81 ... Time-of-flight mass spectrometer, 811 ... Sample gas ionization chamber part, 812 ... Mass spectrometer tube part, 8121 ... Mass gate, 8122 ... Reflective electrode group, 8123 ... Microchannel plate, 817 ... YAG Laser oscillator, 818 ... wavelength variable system.

Claims (10)

  The detected member is allowed to contain a tag gas of a predetermined composition, the composition of the tag gas released when the detected member is damaged is measured, and the amount of change in the composition is calculated. A method for measuring the amount of neutron irradiation characterized by determining the amount of neutron irradiation up to   In claim 1, when detecting damage and neutron irradiation amount of a plurality of detected members, tag materials having different specific compositions are included in each detected member, and these detected members are placed in a furnace to emit radiation. Irradiation is performed, the composition of the tag gas released when the detected member is damaged is measured, and the amount of change in the composition is calculated, thereby identifying the damaged detected member and the neutron irradiation amount of the detected member. A method for measuring a neutron dose, characterized in that it is obtained.   3. The neutron irradiation measurement method according to claim 1, wherein the amount of change in the composition of the tag gas is obtained by calculating a change in the ratio of two predetermined isotopes. 4. The neutron irradiation measurement method according to claim 3, wherein the two predetermined isotopes are ¹²⁹ Xe and ¹³⁰ Xe, and the ratio is ¹³⁰ Xe / ¹²⁹ Xe.   The fuel rods installed in the nuclear reactor are divided into multiple groups, one with the same replacement period, and the tag gas sealed in the fuel rods (in the fuel cladding tube) in each group is released when the fuel rods are damaged. By changing the composition so that it can be identified within each group by measuring and identifying the composition, the fuel rods in each group are identified by the composition of the tag gas released when the fuel rod is broken, The identification of which group of fuel rods is obtained by calculating the amount of change in the composition of the released tag gas to obtain the neutron irradiation amount from when the fuel rod was mounted, and based on this neutron irradiation amount, the mounting time ( A nuclear fuel damage detection method, characterized in that it is carried out by seeking the replacement time.   6. The nuclear fuel damage detection method according to claim 5, wherein the measurement of the composition of the tag gas released when the fuel rod is broken is performed by sampling the cover gas of the nuclear reactor.   A gas sampling device that samples the tag gas released when the detected member is damaged, a tag gas measurement device that measures the composition of the sampled tag gas, calculates the amount of change in the measured composition, and is detected based on the amount of change A device for measuring a neutron dose, comprising means for obtaining a dose of neutron that causes damage to a member.   A gas sampling device that samples the tag gas released when the member to be detected breaks, a tag gas measurement device that measures the composition of the sampled tag gas, calculates the amount of change in the measured composition, and breaks based on the measured composition A neutron irradiation dose measuring apparatus comprising means for identifying a detected member and determining a neutron irradiation dose that leads to breakage of the detected member based on a change amount. When the fuel rods to be mounted are divided into a plurality of groups having the same replacement period as one group, the tag gas sealed in the fuel rods (in the fuel cladding tube) in each group is released when the fuel rods are broken and released. In the reactor of the configuration changed so that identification within each group can be performed by measuring and identifying its composition,
A gas sampling device that samples the tag gas released when the fuel rod is broken; a tag gas measurement device that measures the composition of the sampled tag gas;
A nuclear fuel failure detection device comprising means for identifying fuel rods in each group according to the measured tag gas composition, calculating a change amount of the measured composition, and identifying a damaged group based on the measured composition .   Resonance excitation and ionization are performed by irradiating the introduced sampling gas with laser light, a tag gas ion beam is formed by passing the mass gate in the form of an ion beam by the control electrode group, and a tag gas ion beam is reflected by the reflection electrode group. A measuring apparatus configured to reach a microchannel plate in ascending order of mass of atoms (molecules) and convert it into a mass spectrum signal.

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