CN113571213A - Method for detecting integrity of neptunium target in irradiation process - Google Patents
Method for detecting integrity of neptunium target in irradiation process Download PDFInfo
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- CN113571213A CN113571213A CN202110698487.5A CN202110698487A CN113571213A CN 113571213 A CN113571213 A CN 113571213A CN 202110698487 A CN202110698487 A CN 202110698487A CN 113571213 A CN113571213 A CN 113571213A
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- 229910052781 Neptunium Inorganic materials 0.000 title claims abstract description 66
- LFNLGNPSGWYGGD-UHFFFAOYSA-N neptunium atom Chemical compound [Np] LFNLGNPSGWYGGD-UHFFFAOYSA-N 0.000 title claims abstract description 66
- 238000000034 method Methods 0.000 title claims abstract description 44
- 230000008569 process Effects 0.000 title claims abstract description 18
- 239000002826 coolant Substances 0.000 claims abstract description 45
- 230000000694 effects Effects 0.000 claims abstract description 29
- 230000004992 fission Effects 0.000 claims abstract description 12
- 238000005259 measurement Methods 0.000 claims description 41
- 238000005070 sampling Methods 0.000 claims description 34
- 230000002159 abnormal effect Effects 0.000 claims description 19
- 238000001228 spectrum Methods 0.000 claims description 12
- 230000008859 change Effects 0.000 claims description 8
- 230000005856 abnormality Effects 0.000 claims description 2
- 230000000737 periodic effect Effects 0.000 claims description 2
- 238000010998 test method Methods 0.000 claims 1
- 238000002474 experimental method Methods 0.000 abstract description 9
- 238000004519 manufacturing process Methods 0.000 abstract description 8
- 238000001514 detection method Methods 0.000 abstract description 7
- 238000011160 research Methods 0.000 abstract description 5
- 238000011156 evaluation Methods 0.000 abstract description 2
- 238000012986 modification Methods 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- 238000012544 monitoring process Methods 0.000 description 2
- 238000012545 processing Methods 0.000 description 2
- 230000002285 radioactive effect Effects 0.000 description 2
- 238000012795 verification Methods 0.000 description 2
- 230000000747 cardiac effect Effects 0.000 description 1
- 238000005253 cladding Methods 0.000 description 1
- 238000012790 confirmation Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000002950 deficient Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C17/00—Monitoring; Testing ; Maintaining
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01T—MEASUREMENT OF NUCLEAR OR X-RADIATION
- G01T1/00—Measuring X-radiation, gamma radiation, corpuscular radiation, or cosmic radiation
- G01T1/16—Measuring radiation intensity
- G01T1/17—Circuit arrangements not adapted to a particular type of detector
- G01T1/178—Circuit arrangements not adapted to a particular type of detector for measuring specific activity in the presence of other radioactive substances, e.g. natural, in the air or in liquids such as rain water
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
- G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
- G21G1/02—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes in nuclear reactors
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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
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Abstract
The invention relates to a method for detecting the integrity of a neptunium target in an irradiation process. By adopting the method for detecting the integrity of the neptunium target in the irradiation process, provided by the invention, the activity concentration of fission product gamma nuclide in the target coolant can be monitored and analyzed in an online mode and an offline mode, so that the aim of effectively judging the integrity of the neptunium target in the reactor is fulfilled, the safety of the neptunium target in the irradiation experiment and production process is ensured, and the safety and the stability of the operation of the reactor are also ensured. The detection method is successfully applied to the irradiation experiment of the neptunium target in the advanced Chinese research, has an important reference value for the subsequent safety evaluation of the neptunium target in-pile irradiation, and provides a method reference for the integrity detection of other targets.
Description
Technical Field
The invention belongs to the field of radioisotope radiation production, and relates to a method for detecting the integrity of a neptunium target in an irradiation process.
Background
The radioisotope battery is a device for converting heat energy released in the decay process of a radioisotope into electric energy through a thermocouple, has the characteristics of small size, light weight, stable and reliable performance, long service life, good environmental tolerance and the like, and has been successfully applied to the fields of spacecrafts, cardiac pacemakers and some special military affairs. The radioactive isotope is used as energy source of radioactive isotope battery, and is more frequently used for releasing alpha particles in decay238Pu、210Po, etc., wherein238Pu is the preferred nuclide for current radioisotope batteries.
At present, get238The predominant path for Pu is in-reactor pairing237And carrying out irradiation production on the Np target. During production, if the target cladding is defective or damaged, a significant amount of fission products may enter the coolant from the reactor core. Therefore, a set of reliable detection method needs to be established, the integrity of the target in the reactor can be effectively judged, and the safety and stability of the target and the reactor in the production process are guaranteed.
In recent years, the Chinese atomic energy science research institute successively develops two neptunium target irradiation experiments, and the high-throughput research heap in China belongs to an innovative experiment. The integrity of the neptunium target in the irradiation process is detected by monitoring and analyzing the activity concentration of fission product nuclide in the reactor coolant, and meanwhile, the running characteristic parameters of the target are obtained, so that reliable safety analysis research data are provided for the subsequent irradiation production of the target, and the method has important guiding significance. Through operation verification and comparison with on-line analysis data, the sampling detection method provided by the invention is reliable and effective, and can be practically applied to subsequent irradiation experiments and target irradiation production.
Disclosure of Invention
Aiming at the defects in the prior art, the invention aims to provide a method for detecting the integrity of a neptunium target in an irradiation process, so as to establish a set of effective and reliable sampling, measuring and analyzing method, improve the sampling and measuring efficiency, ensure the accuracy of sampling, measuring and analyzing results and provide a method reference for a subsequent target irradiation experiment.
To achieve this object, the present invention provides a method for detecting the integrity of a neptunium target during irradiation, characterized in that it comprises the following steps:
sampling and measuring a background sample: before the reactor is started, sampling and measuring the coolant of the neptunium target at least once to be used as a background sample;
and (II) carrying out online tracking analysis on activity concentration of gamma nuclide in the neptunium target coolant: in the irradiation process of the neptunium target, recording, tracking and analyzing the activity concentration of fission product gamma nuclide in the cooling agent of the neptunium target and the total gamma dose rate of target damage on line;
(III) sampling, off-line measurement and nuclide analysis in reactor irradiation operation: (1) after a reactor is started and during steady-state irradiation operation, under the working condition that the activity concentration of gamma nuclide in the neptunium target coolant has no abnormal change, the neptunium target coolant is periodically sampled, offline measured and analyzed for nuclide; (2) when the results of off-line measurement and nuclide analysis feedback show that the activity concentration of gamma nuclide in the Np target coolant is abnormal, and an on-line tracking analyzer triggers an alarm value, stopping the reactor; (3) the results of off-line measurement and nuclide analysis feedback show that the activity concentration of gamma nuclide in the neptunium target coolant is abnormal, when the on-line tracking analyzer does not trigger an alarm value, the sampling frequency is increased to further confirm, if the activity concentration of gamma nuclide in the neptunium target coolant is determined to be not abnormal through off-line measurement analysis, steady irradiation operation is continued, otherwise, the reactor is stopped; (4) the results of off-line measurement and nuclide analysis feedback show that the activity concentration of gamma nuclide in the neptunium target coolant has no abnormal change, but when an on-line tracking analyzer triggers an alarm value, the sampling frequency is increased to further confirm, if the activity concentration of gamma nuclide in the neptunium target coolant is determined to have no abnormality through off-line measurement analysis, steady irradiation operation is continued, otherwise, the reactor is stopped.
Further, in the step (three) of the detection method, after the reactor is started, if the power step is first increased, the neptunium target coolant is subjected to follow-up sampling once per hour in the process of increasing each power step before reaching the power step of steady-state irradiation operation, and after the results of offline measurement and nuclide analysis feedback show that the activity concentration of gamma nuclide in the neptunium target coolant has no abnormal change, the power step is continuously increased step by step.
Further, the periodic sampling, offline measurement and nuclide analysis of the neptunium target coolant means that the neptunium target coolant is sampled, offline measured and nuclide analyzed once every fixed time interval of 6 to 10 hours.
Further, the sampling container is a sealed flat sampling bag.
Further, the abnormal activity concentration of gamma nuclide in the neptunium target coolant refers to: the abnormal activity concentration of the gamma nuclide in the neptunium target coolant refers to that: two or more typical fission product nuclides are present in the offline measurement and nuclide analysis results.
Further, the typical fission product nuclide is a key characteristic gamma nuclide of any one of Kr, Xe, I, Cs.
Further, after the sampling operation is finished, the taken sample is kept stand for 900-.
Further, the off-line measurement and nuclide analysis comprises the steps of: selecting a fixed active time point within 600-800 seconds after the off-line measurement is started, storing a first gamma energy spectrogram of the measured sample, and performing nuclide analysis with short half-life; eliminating all counts of the first gamma energy spectrum, restarting the measurement, selecting a fixed active time point after 1200-2000 seconds, storing the second gamma energy spectrum of the measured sample, and performing nuclide analysis with a medium time half-life period.
Further, the off-line measurement and nuclide analysis further comprises the following steps: clearing all counts of the second gamma energy spectrum, restarting the measurement after 24 hours, selecting a fixed active time point after 3600-4000 seconds, storing the third gamma energy spectrum of the measured sample, and performing nuclide analysis with longer half-life period.
The method for detecting the integrity of the neptunium target in the irradiation process has the advantages that the method for detecting the integrity of the neptunium target in the irradiation process can monitor and analyze the activity concentration of fission product gamma nuclide in a target coolant in an online mode and an offline mode, so that the aim of effectively judging the integrity of the neptunium target in a reactor is fulfilled, the safety of the neptunium target in the irradiation experiment and production process is guaranteed, and the safety and stability of the operation of the reactor are also guaranteed. The detection method is successfully applied to the irradiation experiment of the neptunium target in the advanced research of China, the successful implementation of the experiment is ensured, and through operation verification and comparison with online analysis data, the sampling, measuring and analyzing method provided by the invention is reliable and effective, has an important reference value for subsequent safety evaluation of neptunium target in-pile irradiation, and provides a method reference for integrity detection of other targets.
Drawings
Fig. 1 is a flow chart of the method for detecting the integrity of the neptunium target in the irradiation process according to the invention.
FIG. 2 is a flow chart of the processing, off-line measurement and nuclide analysis of a sampled test sample according to the present invention.
Detailed Description
The invention is further described with reference to the following figures and detailed description.
As shown in fig. 1, a method for detecting the integrity of a neptunium target during irradiation comprises the following steps:
sampling and measuring a background sample: before the reactor is started, sampling and measuring the neptunium target coolant for three times to be used as a background sample;
and (II) carrying out online tracking analysis on activity concentration of gamma nuclide in the neptunium target coolant: in the irradiation process of the neptunium target, recording, tracking and analyzing the activity concentration of fission product gamma nuclide in the cooling agent of the neptunium target and the total gamma dose rate of target damage on line;
(III) sampling, off-line measurement and nuclide analysis in reactor irradiation operation: (1) after a reactor is started, if the power step is lifted for the first time, before the power step reaches the power step of steady irradiation operation, in the lifting process of each power step, carrying out one-time following sampling on the neptunium target piece coolant by using a sealed flat sampling bag every hour, and after the results of off-line measurement and nuclide analysis feedback show that the activity concentration of gamma nuclide in the neptunium target piece coolant has no abnormal change, continuously lifting the power step by step; (2) during steady-state irradiation operation, under the condition that the activity concentration of gamma nuclide in the neptunium target coolant has no abnormal change, sampling, measuring and nuclide analyzing are carried out on the neptunium target coolant every 8 hours; (3) the results fed back from the off-line measurements and nuclide analysis show that an anomaly in the activity concentration of the gamma nuclide in the np target coolant is present, i.e. two or more of the following typical fission product nuclides are present in the measurement and nuclide analysis results:85mKr、87Kr、131I、135Xe、138when Cs is detected, if the online tracking analyzer also triggers an alarm value, the reactor is stopped; (4) if only one of the following two monitoring results appears: 1) off-line measurement and nuclide analysis feedback results show that the activity concentration of gamma nuclide in the neptunium target coolant is abnormal, 2) an on-line tracking analyzer triggers an alarm value, the sampling frequency is increased to perform off-line measurement and nuclide analysis for further confirmation, if the activity concentration of gamma nuclide in the neptunium target coolant is determined to be not abnormal through multiple sampling measurement analysis, steady irradiation operation is continued, and otherwise, the reactor is stopped.
As shown in fig. 2, in this embodiment, the processing, offline measurement and nuclide analysis of the sampled to-be-measured sample includes the following steps:
firstly, after the sampling operation is finished, the sample to be tested is stood for 1800 seconds, so that the active nuclide with high activity but short service life, such as27Mg (half-life 9.46 minutes) decays to a lower level to reduce interference of the activated product in the coolant;
selecting 720 second of living time to start after the measurement starts, and storing the measured samplePrimarily for analyzing short half-life nuclides, e.g. for87Kr、138Cs, etc.;
removing all counts from the first gamma energy spectrum, restarting measurement, selecting the 1800 th second of the living time to start, and storing the second gamma energy spectrum of the measured sample for analyzing nuclides with medium-time half-life period, such as85mKr, etc.;
eliminating all counts of the second gamma energy spectrum, restarting measurement after 24 hours, selecting the 3900 th second of the active time to start, and storing the third gamma energy spectrum of the measured sample for analyzing nuclides with longer half-life period, such as nuclides with longer half-life period131I、135Xe, and the like.
The above-described embodiments are merely illustrative of the present invention, and those skilled in the art can make various changes and modifications to the present invention without departing from the spirit and scope of the present invention. Thus, if such modifications and variations of the present invention fall within the scope of the claims of the present invention and their equivalents, the present invention is also intended to include such modifications and variations.
Claims (9)
1. A method for detecting the integrity of a neptunium target during irradiation, said method comprising the steps of:
sampling and measuring a background sample: before the reactor is started, sampling and measuring the coolant of the neptunium target at least once to be used as a background sample;
and (II) carrying out online tracking analysis on activity concentration of gamma nuclide in the neptunium target coolant: in the irradiation process of the neptunium target, recording, tracking and analyzing the activity concentration of fission product gamma nuclide in the cooling agent of the neptunium target and the total gamma dose rate of target damage on line;
(III) sampling, off-line measurement and nuclide analysis in reactor irradiation operation: (1) after a reactor is started and during steady-state irradiation operation, under the working condition that the activity concentration of gamma nuclide in the neptunium target coolant has no abnormal change, the neptunium target coolant is periodically sampled, offline measured and analyzed for nuclide; (2) when the results of off-line measurement and nuclide analysis feedback show that the activity concentration of gamma nuclide in the Np target coolant is abnormal, and an on-line tracking analyzer triggers an alarm value, stopping the reactor; (3) the results of off-line measurement and nuclide analysis feedback show that the activity concentration of gamma nuclide in the neptunium target coolant is abnormal, when the on-line tracking analyzer does not trigger an alarm value, the sampling frequency is increased to further confirm, if the activity concentration of gamma nuclide in the neptunium target coolant is determined to be not abnormal through off-line measurement analysis, steady irradiation operation is continued, otherwise, the reactor is stopped; (4) the results of off-line measurement and nuclide analysis feedback show that the activity concentration of gamma nuclide in the neptunium target coolant has no abnormal change, but when an on-line tracking analyzer triggers an alarm value, the sampling frequency is increased to further confirm, if the activity concentration of gamma nuclide in the neptunium target coolant is determined to have no abnormality through off-line measurement analysis, steady irradiation operation is continued, otherwise, the reactor is stopped.
2. The method according to claim 1, wherein in step (iii), after the reactor is started, if the power step is first increased, the neptunium target coolant is subjected to follow-up sampling once per hour during each power step increase before reaching the power step of steady-state irradiation operation, and after the results of off-line measurement and nuclide analysis feedback show that there is no abnormal change in the activity concentration of gamma nuclide in the neptunium target coolant, the power step is continuously increased step by step.
3. A method as claimed in claim 1 or claim 2, wherein the periodic sampling, off-line measurement and nuclide analysis of the np target coolant is performed once every 6 to 10 hours at a fixed time interval.
4. The method according to claim 3, wherein the sampling container is a sealed flat sampling bag.
5. The method for detecting the integrity of the neptunium target in the irradiation process as claimed in claim 3, wherein the abnormal activity concentration of the gamma nuclide in the coolant of the neptunium target is as follows: two or more typical fission product nuclides are present in the offline measurement and nuclide analysis results.
6. A method of testing the integrity of the neptunium target during irradiation as claimed in claim 5 wherein the typical fission product species is a critical gamma species of any of Kr, Xe, I, Cs.
7. The method for detecting the integrity of the neptunium target in the irradiation process as claimed in any one of claims 4-6, wherein after the sampling operation is completed, the off-line measurement is started after the taken sample is left for 900-3600 seconds.
8. The method according to claim 7 for detecting the integrity of the neptunium target during irradiation, wherein the off-line measurement and nuclide analysis comprise the steps of: selecting a fixed active time point within 600-800 seconds after the off-line measurement is started, storing a first gamma energy spectrogram of the measured sample, and performing nuclide analysis with short half-life; eliminating all counts of the first gamma energy spectrum, restarting the measurement, selecting a fixed active time point after 1200-2000 seconds, storing the second gamma energy spectrum of the measured sample, and performing nuclide analysis with a medium time half-life period.
9. The method for detecting the integrity of the neptunium target during irradiation according to claim 8, wherein the off-line measurement and nuclide analysis further comprises the steps of: clearing all counts of the second gamma energy spectrum, restarting the measurement after 24 hours, selecting a fixed active time point after 3600-4000 seconds, storing the third gamma energy spectrum of the measured sample, and performing nuclide analysis with longer half-life period.
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