CN113921150A - Detection method for leakage of solid gadolinium neutron poison rod - Google Patents
Detection method for leakage of solid gadolinium neutron poison rod Download PDFInfo
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- CN113921150A CN113921150A CN202111121336.XA CN202111121336A CN113921150A CN 113921150 A CN113921150 A CN 113921150A CN 202111121336 A CN202111121336 A CN 202111121336A CN 113921150 A CN113921150 A CN 113921150A
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- Prior art keywords
- gadolinium
- neutron poison
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- poison rod
- detecting
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- 239000002574 poison Substances 0.000 title claims abstract description 71
- 231100000614 poison Toxicity 0.000 title claims abstract description 71
- 229910052688 Gadolinium Inorganic materials 0.000 title claims abstract description 68
- UIWYJDYFSGRHKR-UHFFFAOYSA-N gadolinium atom Chemical compound [Gd] UIWYJDYFSGRHKR-UHFFFAOYSA-N 0.000 title claims abstract description 68
- 239000007787 solid Substances 0.000 title claims abstract description 65
- 238000001514 detection method Methods 0.000 title claims abstract description 23
- 239000007788 liquid Substances 0.000 claims abstract description 58
- 238000000034 method Methods 0.000 claims abstract description 51
- 239000012857 radioactive material Substances 0.000 claims abstract description 32
- 239000002915 spent fuel radioactive waste Substances 0.000 claims abstract description 31
- 230000000155 isotopic effect Effects 0.000 claims abstract description 25
- 230000002285 radioactive effect Effects 0.000 claims abstract description 23
- 230000008569 process Effects 0.000 claims abstract description 22
- 238000007689 inspection Methods 0.000 claims abstract description 5
- 238000005070 sampling Methods 0.000 claims abstract description 5
- 230000001681 protective effect Effects 0.000 claims description 15
- 229910052778 Plutonium Inorganic materials 0.000 claims description 9
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 claims description 9
- 239000000463 material Substances 0.000 claims description 6
- 229910001069 Ti alloy Inorganic materials 0.000 claims description 5
- 229910001093 Zr alloy Inorganic materials 0.000 claims description 4
- 238000000605 extraction Methods 0.000 claims description 4
- 238000000926 separation method Methods 0.000 claims 1
- 230000035945 sensitivity Effects 0.000 abstract description 10
- 238000004458 analytical method Methods 0.000 abstract description 6
- 238000012958 reprocessing Methods 0.000 description 3
- 238000005260 corrosion Methods 0.000 description 2
- 230000007797 corrosion Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 206010041662 Splinter Diseases 0.000 description 1
- 229910052770 Uranium Inorganic materials 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000004949 mass spectrometry Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 244000144985 peep Species 0.000 description 1
- 230000000149 penetrating effect Effects 0.000 description 1
- 238000012805 post-processing Methods 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C17/00—Monitoring; Testing ; Maintaining
- G21C17/002—Detection of leaks
-
- 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
Landscapes
- Physics & Mathematics (AREA)
- Engineering & Computer Science (AREA)
- Plasma & Fusion (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Monitoring And Testing Of Nuclear Reactors (AREA)
- Measurement Of Radiation (AREA)
Abstract
The invention discloses a method for detecting leakage of a solid gadolinium neutron poison rod, which comprises the following steps: 1) sampling the radioactive feed liquid; 2) separating gadolinium element in the sample; 3) analyzing and detecting the isotopic abundance of gadolinium-157 in the sample; 4) and in service inspection, repeating the steps 1) -3), and if the isotope abundance of the gadolinium-157 in the sample is higher than a preset operation threshold, judging that the solid gadolinium neutron poison rod in the radioactive material liquid leaks into the radioactive material liquid. The method for detecting leakage of the solid gadolinium neutron poison rod, which is provided by the invention, is based on an analysis method of gadolinium-157 isotope abundance, has the advantages of high detection sensitivity, simplicity in operation, reliability in detection, short time consumption and no need of shutdown, and guarantees the nuclear critical safety of a spent fuel post-treatment process.
Description
Technical Field
The invention belongs to the technical field of radioactivity detection, and particularly relates to a method for detecting leakage of a solid gadolinium neutron poison rod.
Background
Nuclear critical safety is a primary prerequisite for nuclear energy utilization. The use of solid neutron poisons to control fissile material to a subcritical safe state is one of the most common critical control methods. The post-processing source item of the spent fuel has complex composition and high radioactivity level. Wet reprocessing of spent fuel requires the use of dissolvers to dissolve fissile nuclides in the spent fuel assembly. The dissolver uses a solid gadolinium neutron poison rod and a titanium alloy sleeve as a protective sleeve to control the critical reactivity. The solid neutron poison is soaked in a high-temperature, strong-radiation and strong-acid dissolving solution for a long time, so that the protective sleeve has the risk of corrosion and leakage, the critical control effect is weakened, and the nuclear potential safety hazard is brought. Therefore, the solid neutron poison rod needs to be inspected in service to ensure that the solid neutron poison rod has no leakage.
At present, the leakage of a solid gadolinium neutron poison rod in a dissolver is detected by being limited by a strong radiation field, and only the solid gadolinium neutron poison rod can be lifted out of the dissolver and then observed through a camera and a peep window in a hot room, so that the operation is complex, the time consumption is long, the detection reliability and the detection effectiveness are seriously insufficient, and the leakage detection of the solid gadolinium neutron poison in a post-treatment plant can not be accurately and reliably detected only by observation.
Disclosure of Invention
The invention aims to solve the technical problems in the prior art, provides a method for detecting leakage of a solid gadolinium neutron poison rod, has the advantages of high detection sensitivity, simplicity in operation and no need of shutdown, and solves the problems of complex operation, long consumed time, and serious detection reliability and effectiveness in detecting leakage of solid gadolinium neutron poison in the prior art.
The technical scheme adopted for solving the technical problem of the invention is to provide a method for detecting leakage of a solid gadolinium neutron poison rod, which comprises the following steps:
1) sampling radioactive feed liquid, wherein the radioactive feed liquid is in the state of using solid neutron poison to control nuclear critical risk;
2) separating gadolinium element in the sample;
3) analyzing and detecting the isotopic abundance of gadolinium-157 in the sample;
4) and in service inspection, repeating the steps 1) -3), and if the isotope abundance of the gadolinium-157 in the sample is higher than a preset operation threshold, judging that the solid gadolinium neutron poison rod in the radioactive material liquid leaks into the radioactive material liquid. Otherwise, judging that the solid gadolinium neutron poison rod in the radioactive material liquid does not leak into the radioactive material liquid.
Preferably, the radioactive material liquid is uniform radioactive material liquid which contains fissile materials and has nuclear critical risk and is generated in a spent fuel post-treatment process.
Preferably, the equipment used in the spent fuel post-treatment process comprises: the spent fuel dissolver at the head end of the spent fuel post-treatment process, the high-concentration plutonium solution storage tank of the plutonium line secondary cycle and other related equipment needing the control of the critical safety of the solid neutron poison rod exist in other spent fuel post-treatment processes.
Preferably, the method for detecting leakage of a solid gadolinium neutron poison rod further comprises a step i) before the step 4): before the solid gadolinium neutron poison rod is in service, detecting the isotopic abundance of gadolinium-157 in the sample as a background value, wherein the preset operation threshold value in the step 4) is higher than the background value.
Preferably, the preset operation threshold of the isotope abundance of the gadolinium-157 in the step 4) is 2-4 times of the background value of the isotope abundance of the gadolinium-157 in the radioactive feed liquid.
Preferably, the analytical instrument used for detecting the isotopic abundance of gadolinium-157 is an isotopic mass spectrometer, the detection limit of the isotopic abundance of gadolinium-157 is lower than 0.01%, and the precision is higher than 1%.
Preferably, the operation threshold preset in the step 4) is 0.1% -0.6%.
Preferably, the gadolinium element in the sample separated in step 2) is separated by using an extraction chromatographic column.
Preferably, the solid gadolinium neutron poison rod adopts natural gadolinium as a neutron poison, a protective sleeve is arranged outside the solid gadolinium neutron poison rod, and the protective sleeve is used for protecting the solid gadolinium neutron poison rod from separating radioactive feed liquid.
Preferably, the material of the protective sleeve is titanium alloy or zirconium alloy.
The method for detecting leakage of the solid gadolinium neutron poison rod, which is provided by the invention, is based on an analysis method of gadolinium-157 isotope abundance, has the advantages of high detection sensitivity, simplicity in operation, reliability in detection, short time consumption and no need of shutdown, and guarantees the nuclear critical safety of a spent fuel post-treatment process.
Detailed Description
In order that those skilled in the art will better understand the technical solutions of the present invention, the present invention will be further described in detail with reference to the following detailed description.
Embodiments of the present patent are described in detail below, wherein like or similar reference numerals refer to like or similar elements or elements having like or similar functions throughout. The following description of the embodiments is merely exemplary in nature and is in no way intended to limit the present disclosure.
Example 1
The embodiment provides a method for detecting leakage of a solid gadolinium neutron poison rod, which comprises the following steps:
1) sampling the radioactive feed liquid;
2) separating gadolinium element in the sample;
3) analyzing and detecting the isotopic abundance of gadolinium-157 in the sample;
4) and in service inspection, repeating the steps 1) -3), and if the isotope abundance of the gadolinium-157 in the sample is higher than a preset operation threshold, judging that the solid gadolinium neutron poison rod in the radioactive material liquid leaks into the radioactive material liquid. Otherwise, judging that the solid gadolinium neutron poison rod in the radioactive material liquid does not leak into the radioactive material liquid.
The method for detecting leakage of the solid gadolinium neutron poison rod, which is provided by the embodiment, is based on an analysis method of gadolinium-157 isotope abundance, has the advantages of high detection sensitivity, simplicity in operation, reliability in detection, short time consumption and no need of shutdown, and guarantees nuclear critical safety of a spent fuel post-treatment process.
Example 2
The embodiment is leakage detection of a solid gadolinium neutron poison rod in a dissolver of a spent fuel post-treatment plant, and can be used for critical control of uniform dissolving liquid generated by burning and dissolving spent fuel with the burning depth of 20-55 Gwd/tU.
The embodiment provides a method for detecting leakage of a solid gadolinium neutron poison rod, which comprises the following steps:
1) the radioactive material liquid is sampled, and the radioactive material liquid is the case of the radioactive material liquid which uses solid neutron poison to control the nuclear critical risk, and specifically, in the embodiment, a small amount of the dissolving liquid sample, namely the radioactive material liquid, is taken out from the dissolver or the dissolving liquid receiving storage tank through the automatic sampling cabinet.
2) Separating gadolinium element in the sample, and separating by using an extraction chromatographic column. Uranium, plutonium and other splinter elements in the sample are removed through the extraction chromatographic column, so that separated gadolinium elements are obtained, and the interference of homomorphic heteronuclides in mass spectrometry is reduced.
3) Before the solid gadolinium neutron poison rod is in service, the isotope abundance of gadolinium-157 in a sample is detected and used as a background value, and the background value of the isotope abundance of gadolinium-157 is 0.08% -0.2%. Wherein, the isotopic abundance of gadolinium-157 is equal to the atomic number of gadolinium-157/the atomic number of total gadolinium.
4) And analyzing and detecting the isotopic abundance of the gadolinium-157 in the sample.
5) And in service inspection, repeating the steps 1), 2) and 4), and if the isotopic abundance of the gadolinium-157 in the sample is higher than a preset operation threshold, judging that the solid gadolinium neutron poison rod in the radioactive material liquid leaks into the radioactive material liquid. Otherwise, judging that the solid gadolinium neutron poison rod in the radioactive material liquid does not leak into the radioactive material liquid. The preset operation threshold value is higher than the background value, the operation threshold value is determined according to the background value, and the operation threshold value is higher than the background value and needs to be specifically determined according to the source item of the radioactive material liquid.
Preferably, the radioactive material liquid is uniform radioactive material liquid which contains fissile materials and has nuclear critical risk and is generated in a spent fuel post-treatment process. Of course, the radioactive material liquid is also suitable for uniform radioactive material liquid which uses solid neutron poison to control nuclear critical risk in other radioactive material liquids.
Preferably, the equipment used in the spent fuel post-treatment process comprises: the spent fuel dissolver at the head end of the spent fuel post-treatment process, the high-concentration plutonium solution storage tank of the plutonium line secondary cycle and other related equipment needing the control of the critical safety of the solid neutron poison rod exist in other spent fuel post-treatment processes.
It should be noted that the equipment used in the spent fuel reprocessing process in this embodiment includes: a spent fuel dissolver at the head end of a spent fuel reprocessing process.
Preferably, the preset operation threshold of the isotope abundance of the gadolinium-157 in the step 5) is 2-4 times of the background value of the isotope abundance of the gadolinium-157 in the radioactive feed liquid.
It should be noted that, in this embodiment, the preset operation threshold of the isotopic abundance of gadolinium-157 in step 5) is 3 times of the background value of the isotopic abundance of gadolinium-157 in the radioactive material liquid.
Preferably, the analytical instrument used for detecting the isotopic abundance of gadolinium-157 is an isotopic mass spectrometer, the detection limit of the isotopic abundance of gadolinium-157 is lower than 0.01%, and the precision is higher than 1%. The isotope mass spectrometer is manufactured by Sammerfei and is of an Element XR model.
Preferably, the operation threshold preset in the step 5) is 0.1% -0.6%.
It should be noted that, in this embodiment, the operation threshold preset in step 5) is 0.3%.
Preferably, the solid gadolinium neutron poison rod adopts natural gadolinium as a neutron poison, a protective sleeve is arranged outside the solid gadolinium neutron poison rod, and the protective sleeve is used for protecting the solid gadolinium neutron poison rod from separating radioactive feed liquid. The protective sleeve is corrosion-resistant, and neutron poison does not directly contact with radioactive feed liquid. Because the radioactive material liquid has strong corrosivity, the risk of corroding and penetrating the protective sleeve of the neutron poison rod exists.
Preferably, the material of the protective sleeve is titanium alloy or zirconium alloy. The solid gadolinium neutron poison rod in the radioactive feed liquid leaks into the radioactive feed liquid due to the protective sleeve leakage.
The protective sleeve in this embodiment is made of titanium alloy.
In the embodiment, whether the solid gadolinium neutron poison leaks or not is judged by analyzing the isotope abundance of gadolinium-157 in the radioactive feed liquid through the difference of the distribution of gadolinium isotope abundances in the radioactive feed liquid and the neutron poison rod.
Gadolinium-157 in the background of radioactive feed liquid is easy to be consumed by nuclear reaction in a nuclear reactor due to large neutron absorption cross section, and the isotope abundance (usually less than 0.2%) is obviously less than that (15.65%) of natural gadolinium-157. This results in a gadolinium-157 isotopic abundance (Gd-157/total Gd) in the radioactive feed liquid that is significantly higher than the background value once the natural gadolinium, which is a solid neutron poison, is corroded and dissolved into the radioactive feed liquid.
The method for detecting leakage of the solid gadolinium neutron poison rod, which is provided by the embodiment, is based on an analysis method of gadolinium-157 isotope abundance, and has the sensitivity superior to 109cps/ppm, abundance sensitivity of better than 7ppm, detection limit of less than 1ppm, dynamic range of more than 109The method has the advantages of simple operation, short time consumption and no shutdown, and effectively ensures the nuclear critical safety of the spent fuel post-treatment process.
Example 3
This example provides a method for detecting leakage of a solid gadolinium neutron poison rod, which differs from the detection method in example 2 in that:
the radioactive feed liquid is uniform radioactive feed liquid which contains fissile substances and has nuclear critical risk and is generated by a spent fuel post-treatment process. And a high-concentration plutonium solution storage tank for secondary circulation of a plutonium line at the head end of the spent fuel post-treatment process.
In this embodiment, the preset operation threshold of the isotopic abundance of gadolinium-157 in step 5) is 2 times of the background value of the isotopic abundance of gadolinium-157 in the radioactive feed liquid.
It should be noted that, in this embodiment, the operation threshold preset in step 5) is 0.1%.
The protective sleeve in this embodiment is made of zirconium alloy.
The method for detecting leakage of the solid gadolinium neutron poison rod, which is provided by the embodiment, is based on an analysis method of gadolinium-157 isotope abundance, and has the sensitivity superior to 109cps/ppm, abundance sensitivity of better than 7ppm, detection limit of less than 1ppm, dynamic range of more than 109The method has the advantages of simple operation, short time consumption and no shutdown, and effectively ensures the nuclear critical safety of the spent fuel post-treatment process.
Example 4
This example provides a method for detecting leakage of a solid gadolinium neutron poison rod, which differs from the detection method in example 2 in that:
in this embodiment, the preset operation threshold of the isotopic abundance of gadolinium-157 in step 5) is 4 times of the background value of the isotopic abundance of gadolinium-157 in the radioactive feed liquid.
It should be noted that, in this embodiment, the operation threshold preset in step 5) is 0.6%.
The method for detecting leakage of the solid gadolinium neutron poison rod, which is provided by the embodiment, is based on an analysis method of gadolinium-157 isotope abundance, and has the sensitivity superior to 109cps/ppm, abundance sensitivity of better than 7ppm, detection limit of less than 1ppm, dynamic range of more than 109The method has the advantages of simple operation, short time consumption and no shutdown, and effectively ensures the nuclear critical safety of the spent fuel post-treatment process.
It will be understood that the above embodiments are merely exemplary embodiments taken to illustrate the principles of the present invention, which is not limited thereto. It will be apparent to those skilled in the art that various modifications and improvements can be made without departing from the spirit and substance of the invention, and these modifications and improvements are also considered to be within the scope of the invention.
Claims (10)
1. A method for detecting leakage of a solid gadolinium neutron poison rod is characterized by comprising the following steps:
1) sampling the radioactive feed liquid;
2) separating gadolinium element in the sample;
3) analyzing and detecting the isotopic abundance of gadolinium-157 in the sample;
4) and in service inspection, repeating the steps 1) -3), and if the isotope abundance of the gadolinium-157 in the sample is higher than a preset operation threshold, judging that the solid gadolinium neutron poison rod in the radioactive material liquid leaks into the radioactive material liquid.
2. The method for detecting the leakage of the solid gadolinium neutron poison rod according to claim 1, wherein the radioactive material liquid is a homogeneous radioactive material liquid which contains fissile materials and has a nuclear critical risk and is generated by a spent fuel post-treatment process.
3. The method for detecting the leakage of the solid gadolinium neutron poison rod according to claim 2, wherein the equipment used in the post-treatment process of the spent fuel comprises: the spent fuel dissolver at the head end of the spent fuel post-treatment process, the high-concentration plutonium solution storage tank of the plutonium line secondary cycle and other related equipment needing the control of the critical safety of the solid neutron poison rod exist in other spent fuel post-treatment processes.
4. The method for detecting leakage of a solid gadolinium neutron poison rod according to claim 1, further comprising step i) before step 4): before the solid gadolinium neutron poison rod is in service, detecting the isotopic abundance of gadolinium-157 in the sample as a background value, wherein the preset operation threshold value in the step 4) is higher than the background value.
5. The method for detecting leakage of a solid gadolinium neutron poison rod according to claim 4, wherein the preset operation threshold of the isotope abundance of gadolinium-157 in the step 4) is 2-4 times of the background value of the isotope abundance of gadolinium-157 in radioactive feed liquid.
6. The method for detecting leakage of a solid gadolinium neutron poison rod according to claim 1, wherein the analytical instrument used for detecting the isotopic abundance of gadolinium-157 is an isotopic mass spectrometer, the detection limit of the isotopic abundance of gadolinium-157 is lower than 0.01%, and the precision is higher than 1%.
7. The method for detecting the leakage of the solid gadolinium neutron poison rod according to any one of claims 1 to 6, wherein the operation threshold preset in the step 4) is 0.1-0.6%.
8. The method for detecting the leakage of the solid gadolinium neutron poison rod according to any one of claims 1 to 6, wherein the gadolinium element in the separation sample in the step 2) is separated by using an extraction chromatographic column.
9. The method for detecting the leakage of the solid gadolinium neutron poison rod according to any one of claims 1 to 6, wherein the solid gadolinium neutron poison rod adopts natural gadolinium as a neutron poison, and a protective sleeve is arranged outside the solid gadolinium neutron poison rod and used for protecting the solid gadolinium neutron poison rod from radioactive feed liquid.
10. The method of claim 9, wherein the protective sleeve is made of a titanium alloy or a zirconium alloy.
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| CN202111121336.XA CN113921150A (en) | 2021-09-24 | 2021-09-24 | Detection method for leakage of solid gadolinium neutron poison rod |
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