CN114082301B - Separation system, method and detection method for isotope iodine in nuclear power plant coolant - Google Patents
Separation system, method and detection method for isotope iodine in nuclear power plant coolant Download PDFInfo
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- CN114082301B CN114082301B CN202111211693.5A CN202111211693A CN114082301B CN 114082301 B CN114082301 B CN 114082301B CN 202111211693 A CN202111211693 A CN 202111211693A CN 114082301 B CN114082301 B CN 114082301B
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- 239000002826 coolant Substances 0.000 title claims abstract description 123
- 238000000926 separation method Methods 0.000 title claims abstract description 109
- 229910052740 iodine Inorganic materials 0.000 title claims abstract description 98
- ZCYVEMRRCGMTRW-UHFFFAOYSA-N 7553-56-2 Chemical compound [I] ZCYVEMRRCGMTRW-UHFFFAOYSA-N 0.000 title claims abstract description 97
- 239000011630 iodine Substances 0.000 title claims abstract description 97
- 238000001514 detection method Methods 0.000 title claims abstract description 29
- 238000000034 method Methods 0.000 title claims description 23
- 239000012528 membrane Substances 0.000 claims abstract description 80
- 238000005342 ion exchange Methods 0.000 claims abstract description 43
- 230000008929 regeneration Effects 0.000 claims description 53
- 238000011069 regeneration method Methods 0.000 claims description 53
- 150000001768 cations Chemical class 0.000 claims description 35
- 150000001450 anions Chemical class 0.000 claims description 30
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 23
- 230000000155 isotopic effect Effects 0.000 claims description 21
- FOIXSVOLVBLSDH-UHFFFAOYSA-N Silver ion Chemical group [Ag+] FOIXSVOLVBLSDH-UHFFFAOYSA-N 0.000 claims description 14
- 238000011010 flushing procedure Methods 0.000 claims description 12
- 239000003456 ion exchange resin Substances 0.000 claims description 10
- 229920003303 ion-exchange polymer Polymers 0.000 claims description 10
- 229910052732 germanium Inorganic materials 0.000 claims description 5
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 claims description 5
- 239000007788 liquid Substances 0.000 claims description 5
- 239000002699 waste material Substances 0.000 claims description 3
- 238000005259 measurement Methods 0.000 abstract description 21
- KRHYYFGTRYWZRS-BJUDXGSMSA-N ac1l2y5h Chemical compound [18FH] KRHYYFGTRYWZRS-BJUDXGSMSA-N 0.000 abstract description 19
- 230000000694 effects Effects 0.000 abstract description 18
- -1 N-13 Chemical compound 0.000 abstract description 6
- 238000004458 analytical method Methods 0.000 abstract description 6
- 230000002452 interceptive effect Effects 0.000 abstract description 5
- 239000000446 fuel Substances 0.000 description 7
- 230000004888 barrier function Effects 0.000 description 5
- 238000010586 diagram Methods 0.000 description 5
- 150000002500 ions Chemical class 0.000 description 5
- 238000011160 research Methods 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- 238000002347 injection Methods 0.000 description 4
- 239000007924 injection Substances 0.000 description 4
- 230000002285 radioactive effect Effects 0.000 description 4
- 229910052709 silver Inorganic materials 0.000 description 3
- 239000004332 silver Substances 0.000 description 3
- PNDPGZBMCMUPRI-HVTJNCQCSA-N 10043-66-0 Chemical compound [131I][131I] PNDPGZBMCMUPRI-HVTJNCQCSA-N 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- 239000000654 additive Substances 0.000 description 2
- 125000002091 cationic group Chemical group 0.000 description 2
- 230000004992 fission Effects 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 230000005855 radiation Effects 0.000 description 2
- 238000011084 recovery Methods 0.000 description 2
- 238000005070 sampling Methods 0.000 description 2
- 238000007789 sealing Methods 0.000 description 2
- 230000035945 sensitivity Effects 0.000 description 2
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical compound [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 description 2
- 238000005303 weighing Methods 0.000 description 2
- JKFYKCYQEWQPTM-UHFFFAOYSA-N 2-azaniumyl-2-(4-fluorophenyl)acetate Chemical compound OC(=O)C(N)C1=CC=C(F)C=C1 JKFYKCYQEWQPTM-UHFFFAOYSA-N 0.000 description 1
- QJGQUHMNIGDVPM-BJUDXGSMSA-N Nitrogen-13 Chemical compound [13N] QJGQUHMNIGDVPM-BJUDXGSMSA-N 0.000 description 1
- 229910021612 Silver iodide Inorganic materials 0.000 description 1
- 230000005856 abnormality Effects 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000003321 amplification Effects 0.000 description 1
- 125000000129 anionic group Chemical group 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000005255 beta decay Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 230000002596 correlated effect Effects 0.000 description 1
- 238000003745 diagnosis Methods 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- YCKRFDGAMUMZLT-BJUDXGSMSA-N fluorine-18 atom Chemical compound [18F] YCKRFDGAMUMZLT-BJUDXGSMSA-N 0.000 description 1
- 230000005251 gamma ray Effects 0.000 description 1
- 229910052736 halogen Inorganic materials 0.000 description 1
- 150000002367 halogens Chemical class 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 238000011835 investigation Methods 0.000 description 1
- 150000004694 iodide salts Chemical class 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012544 monitoring process Methods 0.000 description 1
- 238000003199 nucleic acid amplification method Methods 0.000 description 1
- ZLMJMSJWJFRBEC-AKLPVKDBSA-N potassium-42 Chemical compound [42K] ZLMJMSJWJFRBEC-AKLPVKDBSA-N 0.000 description 1
- 238000003908 quality control method Methods 0.000 description 1
- 239000000700 radioactive tracer Substances 0.000 description 1
- 229940096017 silver fluoride Drugs 0.000 description 1
- 229940045105 silver iodide Drugs 0.000 description 1
- REYHXKZHIMGNSE-UHFFFAOYSA-M silver monofluoride Chemical compound [F-].[Ag+] REYHXKZHIMGNSE-UHFFFAOYSA-M 0.000 description 1
- 229910001961 silver nitrate Inorganic materials 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D59/00—Separation of different isotopes of the same chemical element
- B01D59/50—Separation involving two or more processes covered by different groups selected from groups B01D59/02, B01D59/10, B01D59/20, B01D59/22, B01D59/28, B01D59/34, B01D59/36, B01D59/38, B01D59/44
-
- 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
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C17/00—Monitoring; Testing ; Maintaining
- G21C17/02—Devices or arrangements for monitoring coolant or moderator
- G21C17/022—Devices or arrangements for monitoring coolant or moderator for monitoring liquid coolants or moderators
-
- 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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- Physics & Mathematics (AREA)
- High Energy & Nuclear Physics (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Plasma & Fusion (AREA)
- Health & Medical Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- General Physics & Mathematics (AREA)
- Molecular Biology (AREA)
- Spectroscopy & Molecular Physics (AREA)
- Measurement Of Radiation (AREA)
Abstract
The application belongs to the field of detection and analysis of radionuclide in a nuclear power plant, and particularly relates to a separation system, a separation method and a detection method of isotope iodine in a coolant of the nuclear power plant; the system comprises: the semi-permeable membrane separation device is used for separating K-42 and N-13 nuclides in the coolant to obtain an intermediate separator; the ion exchange column is used for adsorbing the isotope iodine in the intermediate separator, effectively separating nuclides such as K-42, N-13, F-18 and the like in the primary loop coolant from nuclides interfering with iodine and isotope measurement, solving the problem of timely measuring the iodine and the isotope in the primary loop coolant of the nuclear power plant, and achieving the effect of improving the detection efficiency and timeliness of the iodine and the isotope.
Description
Technical Field
The application belongs to the field of detection and analysis of radionuclide in a nuclear power plant, and particularly relates to a separation system, a separation method and a detection method of isotope iodine in a coolant of the nuclear power plant.
Background
Iodine and its isotopes are the most commonly used tracer nuclides for fuel assembly breakage in nuclear power plants, and have strict limit requirements on the activity of iodine-131 (I-131) nuclides. The radioactive I-131 nuclides entering the primary loop coolant of the nuclear power plant can be released into the air of the reactor plant through quantitative and non-quantitative leakage and the access opening crossing the second safety barrier, thereby bringing internal irradiation risks to staff in the plant. Therefore, the radioactive I-131 nuclides in the primary loop coolant need to be monitored accurately in time to judge the integrity of the fuel assembly so as to ensure the safety of the unit and reduce the risk of personnel operation.
Disclosure of Invention
The utility model provides a separation system, method and detection method of isotope iodine in nuclear power plant's coolant, effectively separate the nuclides of potassium-42 (K-42), nitrogen-13 (N-13), fluorine-18 (F-18) etc. in the loop coolant to iodine and isotope measurement interference's nuclides, solve the problem of iodine and isotope timely measurement in the nuclear power plant's loop coolant, reached the effect that improves iodine and isotope's detection efficiency and timeliness.
The technical scheme for realizing the purpose of the application comprises the following steps:
the first aspect of the present application provides a separation system for isotopic iodine in a nuclear power plant coolant, comprising: a semipermeable membrane separation device and an ion exchange column;
the input end of the semi-permeable membrane separation device is connected with the output end of the coolant, and the output end of the semi-permeable membrane separation device is connected with the input end of the ion exchange column;
the semi-permeable membrane separation device is used for separating K-42 and N-13 nuclides in the coolant to obtain an intermediate separator;
the ion exchange column is used for adsorbing the isotope iodine in the intermediate separation object.
Optionally, the semipermeable membrane separation device comprises: a first semipermeable membrane, a second semipermeable membrane, and an ionization device;
forming three compartments with the first semi-permeable membrane and the second semi-permeable membrane; the three compartments, comprising: a cation regeneration compartment, an anion regeneration compartment, and a sample compartment; the sample compartment is located between the cation regeneration compartment and the anion regeneration compartment;
the ionization device is used for ionizing pure water in the cation regeneration compartment and the anion regeneration compartment respectively, and forming cations and anions in the cation regeneration compartment and the anion regeneration compartment;
the first semi-permeable membrane only allows cations to move from the cation regeneration compartment to the sample compartment; the second semipermeable membrane only allows cations to move from the sample compartment to the anion regeneration compartment;
the coolant flows from one end of the sample compartment to the other, resulting in the intermediate separator.
Optionally, the flow of pure water in the cation regeneration compartment and the anion regeneration compartment is opposite to the flow of coolant in the sample compartment.
Optionally, the semi-permeable membrane separation device further comprises a first pump for feeding the pure water into the cation regeneration compartment and the anion regeneration compartment;
and/or the number of the groups of groups,
the semi-permeable membrane separation device further comprises a second pump for inputting the coolant into the sample compartment.
Optionally, the ion exchange column is specifically a silver ion exchange column.
Optionally, the silver ion exchange column includes: a first baffle, a second baffle, and a silver ion exchange resin disposed between the first baffle and the second baffle;
the first baffle is provided with a sample inlet for inputting the intermediate separator;
the second baffle is provided with a sample outlet for outputting waste liquid;
the silver ion exchange resin is used for adsorbing the isotope iodine.
The second aspect of the application provides a separation method of isotope iodine in a nuclear power plant coolant, which is applied to any separation system of isotope iodine in the nuclear power plant coolant provided in the first aspect of the application; the separation method comprises the following steps:
and inputting a coolant into an input end of the semi-permeable membrane separation device, so that the semi-permeable membrane separation device separates K-42 and N-13 nuclides in the coolant to obtain an intermediate separator, and the ion exchange column adsorbs isotope iodine in the intermediate separator.
Optionally, the inputting of the coolant into the input end of the semi-permeable membrane separation device further comprises:
pre-flushing a separation system of isotope iodine in the nuclear power plant coolant by pure water;
said feeding coolant to the input of said semi-permeable membrane separation device, further comprising:
and flushing the residual coolant of the separation system of the isotope iodine in the coolant of the nuclear power plant by using pure water.
Optionally, the input end for inputting the coolant into the semipermeable membrane separation device specifically includes:
the coolant is fed to the input of the semi-permeable membrane separation device at a flow rate of 1.0 mL/min.
Optionally, the pre-rinse time is 5 minutes; and/or, the time of the flushing is 5 minutes.
The third aspect of the application provides a method for detecting the isotope iodine in the coolant of the nuclear power plant, which is applied to any of the separation systems of the isotope iodine in the coolant of the nuclear power plant provided in the first aspect of the application; the detection method comprises the following steps:
inputting a coolant into an input end of the semi-permeable membrane separation device, so that the semi-permeable membrane separation device separates K-42 and N-13 nuclides in the coolant to obtain an intermediate separator, and the ion exchange column adsorbs isotope iodine in the intermediate separator;
and detecting the isotope iodine adsorbed by the ion exchange column by using a high-purity germanium spectrometer.
The beneficial technical effects of this application lie in:
(1) The application researches and successfully separates the high-activity nuclides of K-42 and N-13 in the form of cations from the I-131 nuclides in a primary loop of a nuclear power plant through a semi-permeable membrane separation device.
(2) The application researches and successfully separates the high-activity nuclides such as F-18 in the primary loop of the nuclear power plant in the form of anions from the I-131 nuclides through an ion exchange column.
(3) The method innovates and adopts a semi-permeable membrane separation device and an ion exchange column series connection process to rapidly separate and enrich I-131 nuclides, designs a separation system of isotope iodine in a nuclear power plant coolant, effectively separates nuclides of K-42, N-13, F-18 and the like in a loop coolant, which interfere with iodine and isotope measurement, realizes timely and accurate monitoring of radioactive I-131 nuclides in the loop coolant, solves the problem of timely measurement of iodine and isotopes in the loop coolant of the nuclear power plant, and achieves the effect of improving the detection efficiency and timeliness of the iodine and the isotopes.
(4) By utilizing the separation system for isotope iodine in the nuclear power plant coolant, the Compton platform of a separated and collected loop sample is reduced by 96%, the detection lower limit of I-131 nuclide is reduced, the detection efficiency of the I-131 nuclide is improved, the purpose of rapidly and accurately detecting the I-131 nuclide is achieved, and the sealing state of a fuel assembly can be timely judged.
(5) The method belongs to the first example at home and abroad, and each index leads the existing domestic analysis method, so that the method has great popularization value and can be widely applied to the field of nuclear power plant radioactivity analysis.
Drawings
Fig. 1 is a schematic structural diagram of a separation system for isotopic iodine in a coolant of a nuclear power plant according to an embodiment of the present application;
FIG. 2 is a schematic structural diagram of a semipermeable membrane separation device according to an embodiment of the present disclosure;
FIG. 3 is a schematic diagram of a specific working principle of a semipermeable membrane separation device according to an embodiment of the present application;
fig. 4 is a schematic diagram of a specific working principle of an ion exchange column according to an embodiment of the present application;
fig. 5 is a schematic structural diagram of a silver ion exchange column according to an embodiment of the present disclosure;
FIG. 6 is a schematic flow chart of a method for separating isotopic iodine from a coolant of a nuclear power plant according to an embodiment of the present application;
fig. 7 is a schematic flow chart of a method for detecting isotopic iodine in a coolant of a nuclear power plant according to an embodiment of the present application.
Fig. 8 is a schematic flow chart of a method for detecting isotopic iodine in a coolant of a nuclear power plant in a specific application scenario according to an embodiment of the present application.
In the figure:
1-a semi-permeable membrane separation device; 11-first semipermeable membrane, 12-second semipermeable membrane, 13-ionization device, 14-cation regeneration compartment, 15-anion regeneration compartment, 16-sample compartment;
2-ion exchange column; 21-a first baffle, 22-a second baffle, 23-silver ion exchange resin, 24-a sample inlet and 25-a sample outlet;
3-a coolant;
81-sample injection bottle; 82-sample pump; 83-current controller; 84-a current controller; 85-semi-permeable membrane separation device; 86-silver ion exchange resin; 87-pure water.
Detailed Description
In order to better understand the present application, a clear and complete description of the technical solutions in the embodiments of the present application will be provided below with reference to the drawings in the embodiments of the present application. It will be apparent that the embodiments described below are only some, but not all, of the embodiments of the present application. All other embodiments, which can be made by a person skilled in the art without the exercise of inventive faculty, are within the scope of protection of the present application, based on the embodiments described herein.
The inventor of the application found in research that in the practice of radionuclide analysis of a coolant, due to different system materials, chemical additives and water quality control modes, certain specific high-activity and high-energy radionuclides exist in a loop coolant, and the high-activity radionuclides spontaneously emit high-intensity rays and generate a high-intensity Compton effect so as to mask the characteristic peak of the low-activity I-131 radionuclides, so that a high-purity germanium gamma spectrometer cannot identify the characteristic peak or measure data abnormality. Through investigation, almost all nuclear power plants in stacks face this common problem.
At present, each nuclear power plant generally takes the extension of sample placement time as a main research direction, reduces the intensity of gamma rays through the natural decay of high-activity radionuclides and short-half-life nuclides so as to reduce the interference of Compton platform peaks, reduce the detection lower limit and improve the detection sensitivity, thereby realizing the measurement of the activity of the I-131 nuclides. However, this method typically requires at least 72 hours of sample placement, and the measurement results are not very time-efficient and do not reflect the changes in I-131 activity in the coolant in a timely manner; in addition, if long-lived high activity interfering species are present, the I-131 species activity will still not be accurately measured.
For this purpose, the inventors of the present application have counted the measured radioactivity data at 100% power of a nuclear power plant unit in order to analyze the nuclides with the greatest influence on the measurement of the I-131 nuclides in a loop coolant, and the average counts of the main radionuclides in a loop coolant are shown in table 1 below.
TABLE 1 primary nuclides of a Nuclear Power plant Unit-Loop
As can be seen from table 1, the high energy rays of a certain nuclear power plant unit are: the energy peak and electron peak of K-42 (half-life 12.36 h) were 26.549% and 71.903%, respectively. By comparison, measured immediately and after 72 hours of standing, it was found that the radiation intensity of both the energy peak and the electron peak of K-42 (half-life 12.36 h) was greatly reduced. The height of the Compton platform is positively correlated with the gamma ray intensity of a loop sample, and according to the analysis result, the main source K-42 and the electron peak which can emit high-intensity gamma rays in the loop coolant sample can make the contribution of the two sources to the Compton platform the greatest and the measurement effect to the I-131 nuclide the greatest.
The electron peak may be generated by the electron pair effect of high energy gamma rays, as well as positrons emitted when beta decay occurs. Through research, it is found that electricityThe main sources of the sub-peaks are N-13 (half-life 9.65 m) and F-18 (half-life 109.77 m), where N-13 is NH 4 + Is present in the cationic state, F-18 being F - Is present in the anionic state.
For this purpose, the inventor realizes K-42 and N-13 (NH) in the primary loop coolant of the nuclear power plant through the semipermeable membrane and the ion exchange column according to the solvent composition of the primary loop coolant, the physical and chemical properties of target nuclides, the separation operation process, laboratory equipment instruments and the like 4 + )、F-18(F - ) And (3) effectively separating the nuclides to improve the detection efficiency of the I-131 nuclides.
According to the embodiment of the application, the interference cause of the nuclear power plant coolant on the measurement of the iodine and the isotopes is fully researched and determined, the method for separating and collecting the iodine and the isotopes is formulated, the nuclides of the K-42, N-13, F-18 and the like in the primary loop coolant interfering with the measurement of the iodine and the isotopes are effectively separated through the semipermeable membrane and the ion exchange column, the problem of timely measurement of the iodine and the isotopes in the primary loop coolant of the nuclear power plant is solved, the purpose of rapidly and accurately measuring the iodine and the isotopes is achieved, and the detection efficiency and timeliness of the iodine and the isotopes are improved.
Based on the foregoing, for clarity and detailed description of the above-described advantages of the present application, a detailed description of the embodiments of the present application will be provided below with reference to the accompanying drawings.
Referring to fig. 1, the structure of a separation and detection system for isotopic iodine in a coolant of a nuclear power plant according to an embodiment of the present application is shown.
The embodiment of the application provides a separation system of isotope iodine in nuclear power plant's coolant, includes: a semipermeable membrane separation device 1 and an ion exchange column 2;
the input end of the semi-permeable membrane separation device 1 is connected with the output end of the coolant 3, and the output end of the semi-permeable membrane separation device 1 is connected with the input end of the ion exchange column 2;
a semipermeable membrane separation device 1 for separating K-42 and N-13 nuclides in the coolant 3 to obtain an intermediate separator;
an ion exchange column 2 for adsorbing the isotopic iodine in the intermediate separator.
The pH control agent of the primary loop of a nuclear power plant unit is KOH, the K-42 nuclide of the coolant is generated by the reaction of K-41 in the KOH and neutrons, and N-13 is mainly fuel U 235 Released after fission and combined with a loop of additive NH 3 After isotope exchange, finally to 13 NH 4 + In the form of a gel. Under normal power operating conditions, the primary coolant is a weakly basic system, the K-42 and N-13 species are present in the primary coolant in a cationic state, while the I-131 species and other radioactive iodides are present in the primary form of anions or elemental iodine. Therefore, the embodiment of the application adopts the semi-permeable membrane separation device 1 to separate cations, anions and iodine simple substance forms to separate K-42 and N-13 nuclides in the coolant, and an intermediate separator is obtained to eliminate the influence of the two nuclides on the measurement of the I-131 nuclide.
It should also be noted that F-18 of a loop of a nuclear power plant unit is mainly fuel U 238 Released after fission and associated with a return impurity F - The ion is subjected to isotope exchange and finally to 18 F - In the form of a gel. Because F and I are halogen, the embodiment of the application adopts a special ion exchange column to separate F-18 and I-131, and the isotope iodine in the intermediate separation is adsorbed to eliminate the influence of F-18 on the measurement of I-131 nuclide.
In practical application, the membrane separation device 1 and the ion exchange column 2 are connected in series, so that the coolant firstly passes through the membrane separation device 1 and then passes through the ion exchange column 2, and the separation of the I-131 and the isotope thereof is finally realized by selecting a proper flow rate.
In some possible implementations of the embodiments of the present application, as shown in fig. 2, the semi-permeable membrane separation device 1 may specifically include: a first semipermeable membrane 11, a second semipermeable membrane 12, and an ionization device 13;
forming three compartments with a first semipermeable membrane 11 and a second semipermeable membrane 12; three compartments, comprising: a cation regeneration compartment 14, an anion regeneration compartment 15 and a sample compartment 16; the sample compartment 16 is located between the cation regeneration compartment 14 and the anion regeneration compartment 15;
ionization means 13 for ionizing pure water in the cation regeneration compartment 14 and the anion regeneration compartment 15, respectively, to form cations and anions in the cation regeneration compartment 14 and the anion regeneration compartment 15;
the first semipermeable membrane 11 allows only the movement of cations from the cation regeneration compartment 14 to the sample compartment 16; the second semipermeable membrane 12 allows only cations to move from the sample compartment 16 to the anion regeneration compartment 15;
the coolant 3 flows from one end to the other end of the inter-sample space 16, resulting in an intermediate separator.
It should be noted that, referring to fig. 3, the specific working principle of the semipermeable membrane separation device provided in the embodiment of the present application is as follows:
the working electrode of the ionization device 13 may be placed in the direction of the cation-regenerating compartment 14 and the anion-regenerating compartment 15 along the regeneration channel. When a potential is applied across the electrodes, pure water from the regeneration channel is immediately electrolyzed, forming H in the anion regeneration compartment 15 2 And OH (OH) - Ions, to form O in the cation regeneration compartment 14 2 And H 3 O + Ions. The first semi-permeable membrane 11 allows H 3 O + Ions move from cation regeneration compartment 14 to sample compartment 16 to neutralize OH "ions. Cations (e.g., K) in the inter-sample space 16 are attracted by the potential applied to the cathode + 、NH 4 + ) Passes through the second semipermeable membrane 12 into the anion regeneration compartment 15 and combines with OH "ions on the electrode to maintain electroneutrality. Thus, the separation of the I-131 species from the K-42, N-13 species is achieved by separating the K-42, N-13 species from the intermediate separation from the sample compartment 16 into the anion regeneration compartment 15.
As an example, the flow direction of pure water in the cation regeneration compartment 14 and the anion regeneration compartment 15 is opposite to the flow direction of coolant in the sample compartment 16 to ensure the separation efficiency.
In practice, the semi-permeable membrane separation device 1 further comprises a first pump for feeding pure water into the cation regeneration compartment and the anion regeneration compartment;
and/or the semi-permeable membrane separation device 1 further comprises a second pump for feeding a coolant into the sample compartment.
In some possible implementations of the embodiments of the present application, the ion exchange column 2 may specifically be a silver ion exchange column.
It should be noted that the separation of I-131 and F-18 was performed according to the type of chemical bond of silver halide. Silver fluoride is an ionic bond and is easy to dissolve in water; while silver iodide is a covalent bond and insoluble in water. By utilizing the characteristic, H is + The type ion exchange column is converted into a silver type ion exchange column by utilizing silver nitrate, and after the intermediate separation substance passes through the silver type ion exchange column, I-131 and isotopes thereof are adsorbed, F-18 cannot be adsorbed, as shown in figure 4, so that the separation of I-131 and F-18 is realized.
In some possible implementations of the embodiments of the present application, as shown in fig. 5, a silver-type ion exchange column may specifically include: a first barrier sheet 21, a second barrier sheet 22, and a silver ion exchange resin 23 disposed between the first barrier sheet 21 and the second barrier sheet 22;
the first shutter 21 is provided with a sample inlet 24 for inputting intermediate separators;
the second baffle 22 is provided with a sample outlet 25 for outputting waste liquid;
silver ion exchange resin 23 for adsorbing isotopic iodine.
According to the separation system for the isotope iodine in the nuclear power plant coolant, provided by the embodiment of the application, the K-42, N-13 and F-18 nuclides in the primary loop coolant can be efficiently separated from the I-131 nuclides, so that the high-speed separation sample preparation of the primary loop sample is realized, meanwhile, the separation rate of the K-42, N-13 and F-18 nuclides and the I-131 nuclides is up to more than 99%, the recovery rate of the K-42, N-13 and F-18 nuclides is up to more than 95%, and the recovery rate of the I-131 nuclides is up to more than 95%.
The application of the result reduces the Compton platform in the one-loop sample amplification measurement by more than 96% within 2 hours, shortens the detection time of I-131 from the original 72 hours to 2 hours, improves the detection efficiency of I-131 nuclide, greatly improves the detection sensitivity,the lower limit of detection is of the order of 10 3 Bq/kg reduced to 10 2 Bq/kg shortens the sealing diagnosis time of the fuel assembly by more than 97 percent, and has important significance for the supervision, radiation protection and unit safety of the fuel.
Based on the separation system of the isotope iodine in the nuclear power plant coolant provided by the embodiment, the embodiment of the application also provides a separation method of the isotope iodine in the nuclear power plant coolant, which is applied to any separation system of the isotope iodine in the nuclear power plant coolant provided by the embodiment.
Referring to fig. 6, a flow chart of a method for separating isotopic iodine from a coolant in a nuclear power plant according to an embodiment of the present application is shown.
The method for separating the isotope iodine in the nuclear power plant coolant provided by the embodiment of the application comprises the following steps:
s601: and (3) inputting the coolant into the input end of the semi-permeable membrane separation device, so that the K-42 and N-13 nuclides in the coolant are separated by the semi-permeable membrane separation device to obtain an intermediate separator, and the ion exchange column adsorbs the isotope iodine in the intermediate separator.
It will be appreciated that the specific separation principle may be specifically described with reference to the above embodiments, and will not be described herein.
In practice, the coolant may be fed to the input of the semi-permeable membrane separation device at a flow rate of 1.0 mL/min.
In some possible implementations of the embodiments of the present application, step S601 may further include:
s602: pre-flushing a separation system of isotope iodine in a coolant of a nuclear power plant by pure water;
in one example, the pre-flush time may be 5 minutes.
Step S601 may further include:
s603: and flushing the residual coolant of the separation system of the isotope iodine in the coolant of the nuclear power plant by using pure water.
In one example, the flushing time may be 5 minutes to flush residual nuclides in the flow line of the separation system of the isotope iodine in the coolant of the nuclear power plant, thereby ensuring the detection accuracy.
According to the embodiment of the application, the interference cause of the nuclear power plant coolant on the measurement of the iodine and the isotopes is fully researched and determined, the method for separating and collecting the iodine and the isotopes is formulated, the nuclides of the K-42, N-13, F-18 and the like in the primary loop coolant interfering with the measurement of the iodine and the isotopes are effectively separated through the semipermeable membrane and the ion exchange column, the problem of timely measurement of the iodine and the isotopes in the primary loop coolant of the nuclear power plant is solved, the purpose of rapidly and accurately measuring the iodine and the isotopes is achieved, and the detection efficiency and timeliness of the iodine and the isotopes are improved.
Based on the separation system of the isotope iodine in the nuclear power plant coolant provided by the embodiment, the embodiment of the application also provides a detection method of the isotope iodine in the nuclear power plant coolant, which is applied to any one of the separation systems of the isotope iodine in the nuclear power plant coolant provided by the embodiment.
Referring to fig. 7, the flow chart of a method for detecting isotopic iodine in a coolant of a nuclear power plant according to an embodiment of the present application is shown.
The embodiment of the application provides a detection method of isotope iodine in a nuclear power plant coolant, which comprises the following steps:
s701: inputting a coolant into an input end of a semipermeable membrane separation device, so that the semipermeable membrane separation device separates K-42 and N-13 nuclides in the coolant to obtain an intermediate separator, and adsorbing isotope iodine in the intermediate separator by an ion exchange column;
it will be appreciated that the specific separation principle may be specifically described with reference to the above embodiments, and will not be described herein.
S702: and detecting the isotope iodine adsorbed by the ion exchange column by using a high-purity germanium spectrometer.
In a specific application scenario, as shown in fig. 8, the method for detecting isotopic iodine in a coolant of a nuclear power plant provided in the embodiment of the present application may specifically include:
step 1: flushing of the separation device. Pure water is added into a sample injection bottle 81, a sample pump 82 is started, a current controller 83 is started, a regeneration liquid pump 84 is started, and the pure water 87 is used for flushing the system for more than 5 minutes.
Step 2: the sample pump 82 is turned off, 30mL of the sample to be separated (i.e., the coolant) is poured into the sample bottle 81, and the electronic balance accurately weighs the mass m 0 ，
Step 3: starting a sample pump 82, sampling at a flow rate of about 1.0mL/min, enabling the sample to sequentially pass through a semipermeable membrane separation device 85 and silver ion exchange resin 86, placing a sample injection bottle 81 pipeline into a pure water bottle after sampling for 20min, flushing residual nuclides in a sample flow path pipeline and an electrolyte flow path pipeline, and closing the sample pump 82 and a regeneration liquid pump 84 after 5 min;
step 4: accurately weighing the sample bottle 81 after 20min of sample injection by using an electronic balance 1 The mass difference Δm=m of the two weighings is calculated 0 -m 1 Delta m is the sample preparation quantity of the first loop sample;
step 5: the silver ion exchange resin 86 having adsorbed I-131 is taken out to complete separation of iodine and its isotopes.
Step 6: i-131 and its isotopic activity were measured using a high purity germanium spectrometer.
According to the embodiment of the application, the interference cause of the nuclear power plant coolant on the measurement of the iodine and the isotopes is fully researched and determined, the method for separating and collecting the iodine and the isotopes is formulated, the nuclides of the K-42, N-13, F-18 and the like in the primary loop coolant interfering with the measurement of the iodine and the isotopes are effectively separated through the semipermeable membrane and the ion exchange column, the problem of timely measurement of the iodine and the isotopes in the primary loop coolant of the nuclear power plant is solved, the purpose of rapidly and accurately measuring the iodine and the isotopes is achieved, and the detection efficiency and timeliness of the iodine and the isotopes are improved.
While the present application has been described in detail with reference to the drawings and the embodiments, the present application is not limited to the above embodiments, and various changes can be made within the knowledge of one of ordinary skill in the art without departing from the spirit of the present application. None of the details described in this application may be prior art.
Claims (10)
1. A separation system for isotope iodine in a nuclear power plant coolant, which is characterized in that: the system comprises: a semipermeable membrane separation device and an ion exchange column;
the input end of the semi-permeable membrane separation device is connected with the output end of the coolant, and the output end of the semi-permeable membrane separation device is connected with the input end of the ion exchange column;
the semi-permeable membrane separation device is used for separating K-42 and N-13 nuclides in the coolant to obtain an intermediate separator;
the ion exchange column is used for adsorbing the isotope iodine in the intermediate separator;
the semipermeable membrane separation device comprises: a first semipermeable membrane, a second semipermeable membrane, and an ionization device;
forming three compartments with the first semi-permeable membrane and the second semi-permeable membrane; the three compartments, comprising: a cation regeneration compartment, an anion regeneration compartment, and a sample compartment; the sample compartment is located between the cation regeneration compartment and the anion regeneration compartment;
the ionization device is used for ionizing pure water in the cation regeneration compartment and the anion regeneration compartment respectively, and forming cations and anions in the cation regeneration compartment and the anion regeneration compartment;
the first semi-permeable membrane only allows cations to move from the cation regeneration compartment to the sample compartment; the second semipermeable membrane only allows cations to move from the sample compartment to the anion regeneration compartment;
the coolant flows from one end of the sample compartment to the other, resulting in the intermediate separator.
2. The separation system of isotopic iodine in a nuclear power plant coolant of claim 1, wherein: the flow of pure water in the cation regeneration compartment and the anion regeneration compartment is opposite to the flow of coolant in the sample compartment.
3. The separation system of isotopic iodine in a nuclear power plant coolant of claim 1, wherein:
the semipermeable membrane separation device further comprises a first pump for inputting the pure water into the cation regeneration compartment and the anion regeneration compartment;
and/or the number of the groups of groups,
the semi-permeable membrane separation device further comprises a second pump for inputting the coolant into the sample compartment.
4. The separation system of isotopic iodine in a nuclear power plant coolant of claim 1, wherein: the ion exchange column is specifically a silver ion exchange column.
5. The separation system of isotopic iodine in a nuclear power plant coolant of claim 4, wherein: the silver ion exchange column comprises: a first baffle, a second baffle, and a silver ion exchange resin disposed between the first baffle and the second baffle;
the first baffle is provided with a sample inlet for inputting the intermediate separator;
the second baffle is provided with a sample outlet for outputting waste liquid;
the silver ion exchange resin is used for adsorbing the isotope iodine.
6. A separation method of isotope iodine in a nuclear power plant coolant is characterized by comprising the following steps: a separation system for isotopic iodine used in the coolant of a nuclear power plant as claimed in any one of claims 1 to 5; the separation method comprises the following steps:
and inputting a coolant into an input end of the semi-permeable membrane separation device, so that the semi-permeable membrane separation device separates K-42 and N-13 nuclides in the coolant to obtain an intermediate separator, and the ion exchange column adsorbs isotope iodine in the intermediate separator.
7. The method for separating isotopic iodine in a coolant of a nuclear power plant according to claim 6, wherein: said feeding coolant to the input of said semi-permeable membrane separation device further comprises:
pre-flushing a separation system of isotope iodine in the nuclear power plant coolant by pure water;
said feeding coolant to the input of said semi-permeable membrane separation device, further comprising:
and flushing the residual coolant of the separation system of the isotope iodine in the coolant of the nuclear power plant by using pure water.
8. The method for separating isotopic iodine in a coolant of a nuclear power plant according to claim 6, wherein: the input end for inputting the coolant into the semi-permeable membrane separation device specifically comprises:
the coolant is fed to the input of the semi-permeable membrane separation device at a flow rate of 1.0 mL/min.
9. The method for separating isotopic iodine in a coolant of a nuclear power plant according to claim 7, wherein: the pre-rinse time is 5 minutes; and/or, the time of the flushing is 5 minutes.
10. A detection method of isotope iodine in a nuclear power plant coolant is characterized by comprising the following steps of: a separation system for isotopic iodine used in the coolant of a nuclear power plant as claimed in any one of claims 1 to 5; the detection method comprises the following steps:
inputting a coolant into an input end of the semi-permeable membrane separation device, so that the semi-permeable membrane separation device separates K-42 and N-13 nuclides in the coolant to obtain an intermediate separator, and the ion exchange column adsorbs isotope iodine in the intermediate separator;
and detecting the isotope iodine adsorbed by the ion exchange column by using a high-purity germanium spectrometer.
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