CN114082301A - 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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- CN114082301A CN114082301A CN202111211693.5A CN202111211693A CN114082301A CN 114082301 A CN114082301 A CN 114082301A CN 202111211693 A CN202111211693 A CN 202111211693A CN 114082301 A CN114082301 A CN 114082301A
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- 239000002826 coolant Substances 0.000 title claims abstract description 124
- 238000000926 separation method Methods 0.000 title claims abstract description 118
- 229910052740 iodine Inorganic materials 0.000 title claims abstract description 100
- ZCYVEMRRCGMTRW-UHFFFAOYSA-N 7553-56-2 Chemical compound [I] ZCYVEMRRCGMTRW-UHFFFAOYSA-N 0.000 title claims abstract description 99
- 239000011630 iodine Substances 0.000 title claims abstract description 99
- 238000001514 detection method Methods 0.000 title claims abstract description 27
- 238000000034 method Methods 0.000 title claims description 23
- 239000012528 membrane Substances 0.000 claims abstract description 78
- 238000005342 ion exchange Methods 0.000 claims abstract description 43
- 230000008929 regeneration Effects 0.000 claims description 54
- 238000011069 regeneration method Methods 0.000 claims description 54
- 150000001768 cations Chemical class 0.000 claims description 37
- 150000001450 anions Chemical class 0.000 claims description 31
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 23
- 239000000126 substance Substances 0.000 claims description 16
- 238000011010 flushing procedure Methods 0.000 claims description 10
- 239000003456 ion exchange resin Substances 0.000 claims description 10
- 229920003303 ion-exchange polymer Polymers 0.000 claims description 10
- 229910052709 silver Inorganic materials 0.000 claims description 10
- 239000004332 silver Substances 0.000 claims description 10
- NWUYHJFMYQTDRP-UHFFFAOYSA-N 1,2-bis(ethenyl)benzene;1-ethenyl-2-ethylbenzene;styrene Chemical compound C=CC1=CC=CC=C1.CCC1=CC=CC=C1C=C.C=CC1=CC=CC=C1C=C NWUYHJFMYQTDRP-UHFFFAOYSA-N 0.000 claims description 9
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 8
- 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
- 238000005406 washing Methods 0.000 claims 1
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- KRHYYFGTRYWZRS-BJUDXGSMSA-N ac1l2y5h Chemical compound [18FH] KRHYYFGTRYWZRS-BJUDXGSMSA-N 0.000 abstract description 19
- 230000000694 effects Effects 0.000 abstract description 17
- 238000004458 analytical method Methods 0.000 abstract description 6
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- PNDPGZBMCMUPRI-HVTJNCQCSA-N 10043-66-0 Chemical compound [131I][131I] PNDPGZBMCMUPRI-HVTJNCQCSA-N 0.000 description 2
- 239000000654 additive Substances 0.000 description 2
- 125000000129 anionic group Chemical group 0.000 description 2
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- 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
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- 229910052736 halogen Inorganic materials 0.000 description 1
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- ZLMJMSJWJFRBEC-AKLPVKDBSA-N potassium-42 Chemical compound [42K] ZLMJMSJWJFRBEC-AKLPVKDBSA-N 0.000 description 1
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- 229940045105 silver iodide Drugs 0.000 description 1
- REYHXKZHIMGNSE-UHFFFAOYSA-M silver monofluoride Chemical compound [F-].[Ag+] REYHXKZHIMGNSE-UHFFFAOYSA-M 0.000 description 1
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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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- General Engineering & Computer Science (AREA)
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- Plasma & Fusion (AREA)
- Health & Medical Sciences (AREA)
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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: a semipermeable membrane separation device 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 in the primary circuit coolant, wherein the nuclides interfere with iodine and isotope measurement by K-42, N-13, F-18 and other nuclides, solves the problem of timely measurement of iodine and isotope in the primary circuit coolant of the nuclear power plant, and achieves the effect of improving the detection efficiency and timeliness of iodine and isotope.
Description
Technical Field
The application belongs to the field of detection and analysis of nuclear power plant radionuclides, and particularly relates to a separation system, a separation method and a detection method of isotope iodine in a nuclear power plant coolant.
Background
Iodine and its isotopes are tracer nuclides for breakage of the most common fuel assemblies used in nuclear power plants, and have strict limit requirements on the activity of the iodine-131 (I-131) nuclide. The radioactive I-131 nuclide entering the primary coolant of the nuclear power plant can be released into the air of the reactor plant through quantitative and non-quantitative leakage and the overhaul opening to pass through the second safety barrier, so that internal irradiation risks are brought to workers in the plant. Therefore, there is a need for timely and accurate monitoring of the radioactive I-131 species in the primary coolant to determine the integrity of the fuel assemblies, to ensure unit safety and to reduce personnel operational risks.
Disclosure of Invention
The purpose of the application is to provide a separation system, a separation method and a detection method for isotope iodine in a nuclear power plant coolant, which are used for effectively separating nuclides such as potassium-42 (K-42), nitrogen-13 (N-13), fluorine-18 (F-18) and the like in a primary loop coolant from nuclides interfering with iodine and isotope measurement, solving the problem of timely measuring iodine and isotope in the primary loop coolant of the nuclear power plant and achieving the effects of improving the detection efficiency and timeliness of iodine and isotope.
The technical scheme for realizing the purpose of the application is as follows:
the application provides in a first aspect a separation system of isotope iodine in nuclear power plant's coolant, includes: 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 isotope iodine in the intermediate separator.
Optionally, the semi-permeable membrane separation device comprises: a first semi-permeable membrane, a second semi-permeable membrane and an ionization device;
forming three compartments with the first and second semi-permeable membranes; the three compartments, including: 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 respectively ionizing pure water in the cation regeneration interval and the anion regeneration interval to form cations and anions in the cation regeneration interval and the anion regeneration interval;
the first semi-permeable membrane only allows cations to move from the cation regeneration compartment to the sample compartment; the second semi-permeable 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 separation.
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 semipermeable membrane separation apparatus further comprises a first pump for feeding the pure water into the cation regeneration compartment and the anion regeneration compartment;
and/or the presence of a gas in the gas,
the semipermeable membrane separation unit further comprises a second pump for feeding the coolant into the sample compartment.
Optionally, the ion exchange column is specifically a silver-type ion exchange column.
Optionally, the silver-type ion exchange column comprises: the device comprises a first baffle plate, a second baffle plate and silver type ion exchange resin arranged between the first baffle plate and the second baffle plate;
the first baffle plate is provided with a sample inlet for inputting the intermediate separator;
the second baffle is provided with a sample outlet and is used for outputting waste liquid;
the silver type 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 coolant of a nuclear power plant, which is applied to any separation system of isotope iodine in the coolant of the nuclear power plant provided by the first aspect of the application; the separation method comprises the following steps:
inputting a coolant into the 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 separated substance, and adsorbing isotope iodine in the intermediate separated substance by the ion exchange column.
Optionally, the inputting of the coolant into the input end of the semipermeable membrane separation device further comprises:
pre-flushing a separation system of isotope iodine in the nuclear power plant coolant by using pure water;
the input end for inputting the coolant into the semi-permeable membrane separation device further comprises:
and flushing the residual coolant of the isotope iodine separation system in the coolant of the nuclear power plant by using pure water.
Optionally, the input of the coolant to the semi-permeable membrane separation device specifically includes:
the coolant was fed to the input of the semipermeable membrane separation unit at a flow rate of 1.0 mL/min.
Optionally, the pre-rinsing time is 5 minutes; and/or the time of the rinsing is 5 minutes.
The third aspect of the application provides a method for detecting isotope iodine in a coolant of a nuclear power plant, which is applied to any one of the separation systems for isotope iodine in the coolant of the nuclear power plant provided by 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 separated substance, and the ion exchange column adsorbs isotope iodine in the intermediate separated substance;
and detecting the isotope iodine adsorbed by the ion exchange column by using a high-purity germanium spectrometer.
The beneficial technical effect of this application lies in:
(1) the application researches and successfully separates K-42 and N-13 in a loop of a nuclear power plant from I-131 nuclide rapidly in the form of cation by a semipermeable membrane separation device.
(2) The application researches and successfully separates the high-activity nuclide existing in the form of anion, such as F-18 and the like in a loop of a nuclear power plant from the I-131 nuclide rapidly through an ion exchange column.
(3) The I-131 nuclide is quickly separated and enriched by adopting a semipermeable membrane separation device and an ion exchange column series connection process, the separation system of the isotope iodine in the nuclear power plant coolant is designed, nuclides such as K-42, N-13 and F-18 in a primary loop coolant and the like which interfere with iodine and isotope measurement are effectively separated, timely and accurate monitoring on the radioactive I-131 nuclide in the primary loop coolant is realized, the problem of timely measurement of the iodine and the isotope in the primary loop coolant in the nuclear power plant is solved, and the effects of improving the detection efficiency and the timeliness of the iodine and the isotope are achieved.
(4) By utilizing the separation system for isotope iodine in the nuclear power plant coolant, the loop sample Compton platform for separation and collection is reduced by 96%, the detection lower limit of the I-131 nuclide is reduced, the efficiency of the I-131 nuclide detection is improved, the purpose of rapidly and accurately detecting the I-131 nuclide is achieved, and the sealing state of the fuel assembly can be timely judged.
(5) The method belongs to the first case at home and abroad, and each index of the method is ahead of the existing domestic analysis method, so that the method has great popularization value and can be widely applied to the field of radioactivity analysis of nuclear power plants.
Drawings
Fig. 1 is a schematic structural diagram of a separation system for isotope iodine in a coolant of a nuclear power plant according to an embodiment of the present disclosure;
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 illustrating the operation principle of a semipermeable membrane separation device according to an embodiment of the present invention;
FIG. 4 is a schematic diagram illustrating the specific operation principle of an ion exchange column according to an embodiment of the present disclosure;
FIG. 5 is a schematic structural diagram of a silver-type ion exchange column according to an embodiment of the present disclosure;
fig. 6 is a schematic flow chart illustrating a method for separating isotope iodine in a coolant of a nuclear power plant according to an embodiment of the present disclosure;
fig. 7 is a schematic flowchart of a method for detecting isotope iodine in a coolant of a nuclear power plant according to an embodiment of the present disclosure.
Fig. 8 is a schematic flow chart of a method for detecting isotope iodine in a coolant of a nuclear power plant according to an embodiment of the present disclosure in a specific application scenario.
In the figure:
1-a semi-permeable membrane separation device; 11-a first semi-permeable membrane, 12-a second semi-permeable membrane, 13-an ionization device, 14-a cation regeneration compartment, 15-an anion regeneration compartment and 16-a sample compartment;
2-ion exchange column; 21-first baffle, 22-second baffle, 23-silver ion exchange resin, 24-sample inlet, 25-sample outlet;
3-a coolant;
81-sample introduction bottle; 82-sample pump; 83-current controller; 84-a current controller; 85-semipermeable membrane separation unit; 86-silver type ion exchange resin; 87-pure water.
Detailed Description
In order to make the technical solutions in the embodiments of the present application more comprehensible to those skilled in the art, the following description will be made in detail and completely with reference to the accompanying drawings in the embodiments of the present application. It should be apparent that the embodiments described below are only some of the embodiments of the present application, and not all of them. All other embodiments that can be derived by a person skilled in the art from the embodiments described herein without inventive step are within the scope of the present application.
The inventor of the present application finds in research that, in the practice of radioactive nuclide analysis of coolant, due to different system materials, chemical additives and water quality control modes, certain specific high-activity and high-energy radioactive nuclides exist in the primary loop coolant, and these high-activity nuclides can spontaneously emit high-intensity rays and generate a high-intensity compton effect, so that the characteristic peak of the low-activity I-131 nuclide is masked, and the high-purity germanium gamma spectrometer cannot identify the characteristic peak or measure data abnormality. By investigation, almost all nuclear power plants of the heap type 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 interference of a Compton platform peak by reducing the intensity of gamma rays through the natural decay of a high-activity radionuclide and a short half-life nuclide, reduces the lower detection limit, and improves the detection sensitivity, thereby realizing the measurement of the activity of the I-131 nuclide. However, this method usually requires the sample to be left for at least 72 hours, and the measurement results are not good in timeliness and cannot reflect the activity change of I-131 in the coolant in time; in addition, if there are long-lived high activity interfering species, the activity of the I-131 species will still not be accurately measured.
Therefore, in order to analyze the nuclide which has the greatest influence on the measurement of the I-131 nuclide in the primary coolant, the inventor of the application carries out statistics on the measured radioactivity data of a certain nuclear power plant unit under the condition of 100% power, and the average count of the main radionuclides in the primary coolant is shown in the following table 1.
TABLE 1 Primary nuclear nuclide of a nuclear power plant
As can be seen from table 1, the high-energy radiation of a certain nuclear power plant unit is: the energy peak and the electron peak of K-42 (half-life period of 12.36h) account for 26.549% and 71.903% respectively. By comparing the measurement immediately and the measurement after 72 hours of standing, the radiation intensity of the energy peak and the electron peak of K-42 (half-life period of 12.36h) is greatly reduced. The height of the Compton platform is positively correlated with the gamma ray intensity of the primary loop sample, and according to the analysis result, the primary loop coolant sample can emit a main source K-42 and an electron peak of high-intensity gamma rays, and the two source terms have the largest contribution to the Compton platform and the largest influence on the I-131 nuclide measurement.
The generation of the electron peak may be the electron pair effect of high energy gamma rays, and the positron emission when beta decay occurs. The main source terms of the electron peaks were found by investigation to be N-13 (half-life 9.65m) and F-18 (half-life 109.77m), where N-13 is NH4 +In the cationic state of (A), F-18 is present as F-Exists in an anionic state.
The inventor of the application realizes the purpose of carrying out the separation on K-42 and N-13 (NH) in the primary coolant through a semipermeable membrane and an ion exchange column according to the conditions of solvent composition of the primary coolant in the nuclear power plant, physicochemical properties of target nuclide, separation operation process, laboratory equipment and instruments and the like4 +)、F-18(F-) Effective separation of the species to improve the detection efficiency of the I-131 species.
According to the embodiment of the application, the interference reasons of the coolant of the nuclear power plant on the measurement of the iodine and the isotope thereof are determined through sufficient research, the method for separating and collecting the iodine and the isotope thereof is formulated, the nuclides of K-42, N-13, F-18 and the like in the coolant of the primary loop are effectively separated through the semipermeable membrane and the ion exchange column, and the nuclides interfering the measurement of the iodine and the isotope thereof are solved, so that the problem of timely measurement of the iodine and the isotope thereof in the coolant of the primary loop of the nuclear power plant is solved, the purpose of quickly and accurately measuring the iodine and the isotope thereof is achieved, and the detection efficiency and timeliness of the iodine and the isotope are improved.
Based on the above, in order to clearly and specifically explain the above advantages of the present application, the following description of the embodiments of the present application will be made with reference to the accompanying drawings.
Referring to fig. 1, the figure is a schematic structural diagram of a separation and detection system for isotope iodine in a nuclear power plant coolant according to an embodiment of the present disclosure.
The separation system of isotope iodine in nuclear power plant's coolant that this application embodiment provided includes: a semipermeable membrane separation device 1 and an ion exchange column 2;
the input end of the semipermeable membrane separation device 1 is connected with the output end of the coolant 3, and the output end of the semipermeable 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;
and the ion exchange column 2 is used for adsorbing isotope iodine in the intermediate separation substance.
It is noted that KOH is used as a pH control agent of a primary loop of a nuclear power plant unit, K-42 nuclide of coolant is generated by the reaction of K-41 in KOH and neutrons, and N-13 is mainly fuel U235Released after fission and mixed with a primary additive NH3After isotope exchange is carried out, the product is finally13NH4 +The form exists. Under normal power operation conditions, the primary loop coolant is a weakly alkaline system, the K-42 and N-13 nuclides mainly exist in a cationic state in the primary loop coolant, and the I-131 nuclide and other radioactive iodine mainly exist in an anionic or iodine elementary substance state. Therefore, the embodiment of the application adopts the semi-permeable membrane separation device 1 to separate cations from anions and iodine elementary substance forms to separate K-42 and N-13 nuclides in the coolant to obtain an intermediate separator so as to eliminate the influence of the two nuclides on the measurement of the I-131 nuclide.
It is also noted that F-18 of a primary loop of a nuclear power plant unit is mainly fuel U238Released after fission and mixed with impurities F of the primary circuit-After isotopic exchange of the ions, the ions are finally treated with18F-The form exists. Since F and I are both halogen, the embodiment of the application adopts a special ion exchange column to separate F-18 and I-131, and adsorbs isotope iodine in the intermediate separation substance 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 semipermeable membrane separation device 1 may specifically include: a first semi-permeable membrane 11, a second semi-permeable membrane 12 and an ionization device 13;
three compartments are formed by the first semi-permeable membrane 11 and the second semi-permeable membrane 12; three compartments, comprising: a cation regeneration compartment 14, an anion regeneration compartment 15 and a sample compartment 16; sample compartment 16 is located between cation regeneration compartment 14 and anion regeneration compartment 15;
an ionization device 13 for ionizing pure water in the cation regeneration compartment 14 and the anion regeneration compartment 15 to form cations and anions in the cation regeneration compartment 14 and the anion regeneration compartment 15, respectively;
the first semi-permeable membrane 11 only allows cations to move from the cation regeneration compartment 14 to the sample compartment 16; the second semi-permeable membrane 12 only allows cations to move from the sample compartment 16 to the anion regeneration compartment 15;
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 can be placed in the direction of the regeneration channel between the cation regeneration compartment 14 and the anion regeneration compartment 15. When a potential is applied across the electrodes, pure water from the regeneration channel is immediately electrolyzed to form H in the anion regeneration compartment 152And OH-Ions to form O in the cation regeneration compartment 142And H3O+Ions. The first semi-permeable membrane 11 allows H3O+Ions move from the cation regeneration compartment 14 to the sample compartment 16 to neutralize the OH "ions. Due to potential attraction acting on the cathodeTo draw cations (e.g. K) in the sample compartment 16+、NH4 +) Passes through the second semi-permeable membrane 12 into the anion regeneration compartment 15 to combine with OH "ions on the electrodes to maintain electrical neutrality. Thus, the K-42 and N-13 species in the intermediate separation from the sample compartment 16 are both separated into the anion regeneration compartment 15, and separation of the I-131 species from the K-42 and N-13 species is achieved.
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 the coolant in the sample compartment 16 to ensure the efficiency of the separation.
In specific implementation, the semipermeable membrane separation apparatus 1 further comprises a first pump for feeding pure water into the cation regeneration compartment and the anion regeneration compartment;
and/or, the semipermeable membrane separation unit 1 further comprises a second pump for feeding a coolant into the sample compartment.
In some possible implementations of the present embodiment, the ion exchange column 2 may be a silver-type ion exchange column.
It should be noted that the separation of I-131 and F-18 is performed according to the type of the silver halide chemical bond. Silver fluoride is an ionic bond and is easily soluble in water; whereas silver iodide is a covalent bond and insoluble in water. By utilizing this characteristic, H+The type ion exchange column is converted into a silver type ion exchange column by using silver nitrate, after the intermediate isolate passes through the silver type ion exchange column, I-131 and isotope thereof are adsorbed, F-18 is not adsorbed, as shown in figure 4, and therefore separation of I-131 and F-18 is achieved.
In some possible implementations of the embodiment of the present application, as shown in fig. 5, the silver-type ion exchange column may specifically include: a first barrier rib 21, a second barrier rib 22, and a silver-type ion exchange resin 23 disposed between the first barrier rib 21 and the second barrier rib 22;
the first flap 21 is provided with a sample inlet 24 for the input of an intermediate separator;
the second shutter 22 is provided with a sample outlet 25 for outputting waste liquid;
and silver-type ion exchange resin 23 for adsorbing isotope iodine.
The separation system for isotope iodine in the nuclear power plant coolant provided by the embodiment of the application can efficiently separate K-42, N-13 and F-18 nuclides from I-131 nuclides in a primary loop coolant, realizes high-speed separation and sample preparation of a primary loop sample, and simultaneously ensures that the separation rate of the K-42, N-13 and F-18 nuclides and the I-131 nuclides reaches more than 99%, the recovery rate of the K-42, N-13 and F-18 nuclides reaches more than 95%, and the recovery rate of the I-131 nuclides also reaches more than 95%.
The application of the result reduces the Compton platform in the radiochemical measurement of a loop sample by more than 96% within 2 hours, shortens the detection time of I-131 from the original 72 hours to 2 hours, improves the efficiency of I-131 nuclide detection, greatly improves the detection sensitivity, and reduces the magnitude order of the lower detection limit from 103Bq/kg is reduced to 102Bq/kg, shortens the diagnosis time of the sealing performance of the fuel assembly by over 97 percent, and has important significance on supervision, radiation protection and unit safety of fuel.
Based on the separation system for isotope iodine in the coolant of the nuclear power plant provided by the embodiment, the embodiment of the application further provides a separation method for isotope iodine in the coolant of the nuclear power plant, and the separation method is applied to any separation system for isotope iodine in the coolant of the nuclear power plant provided by the embodiment.
Referring to fig. 6, the figure is a schematic flow chart of a separation method of isotope iodine in a nuclear power plant coolant according to an embodiment of the present application.
The separation method of isotope iodine in the nuclear power plant coolant provided by the embodiment of the application comprises the following steps:
s601: the coolant is input into the input end of the 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 separated substance, and the ion exchange column adsorbs isotope iodine in the intermediate separated substance.
It is to be understood that the specific separation principle can be specifically described with reference to the above embodiments, and is not described herein again.
In practice, the coolant may be fed to the input of the semipermeable membrane separation unit at a flow rate of 1.0 mL/min.
In some possible implementation manners of the embodiment 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 using pure water;
in one example, the time for the pre-flush may be 5 minutes.
Step S601, then, may further include:
s603: and flushing the residual coolant of the isotope iodine separation system in the coolant of the nuclear power plant by using pure water.
In one example, the time for flushing may be 5 minutes, and residual nuclides in a flow line of a separation system for isotope iodine in a coolant of a nuclear power plant are flushed, so that the detection accuracy is ensured.
According to the embodiment of the application, the interference reasons of the coolant of the nuclear power plant on the measurement of the iodine and the isotope thereof are determined through sufficient research, the method for separating and collecting the iodine and the isotope thereof is formulated, the nuclides of K-42, N-13, F-18 and the like in the coolant of the primary loop are effectively separated through the semipermeable membrane and the ion exchange column, and the nuclides interfering the measurement of the iodine and the isotope thereof are solved, so that the problem of timely measurement of the iodine and the isotope thereof in the coolant of the primary loop of the nuclear power plant is solved, the purpose of quickly and accurately measuring the iodine and the isotope thereof is achieved, and the detection efficiency and timeliness of the iodine and the isotope are improved.
Based on the separation system for isotope iodine in the coolant of the nuclear power plant provided by the embodiment, the embodiment of the application further provides a detection method for isotope iodine in the coolant of the nuclear power plant, and the method is applied to any separation system for isotope iodine in the coolant of the nuclear power plant provided by the embodiment.
Referring to fig. 7, the figure is a schematic flow chart of a method for detecting isotope iodine in a nuclear power plant coolant according to an embodiment of the present application.
The method for detecting isotope iodine in the coolant of the nuclear power plant provided by the embodiment of the application comprises the following steps:
s701: inputting the coolant into the input end of the 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 using an ion exchange column;
it is to be understood that the specific separation principle can be specifically described with reference to the above embodiments, and is not described herein again.
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, a method for detecting isotope iodine in a coolant of a nuclear power plant provided in an embodiment of the present application may specifically include:
step 1: and (5) flushing the separation device. Adding pure water into a sample injection bottle 81, starting a sample pump 82, starting a current controller 83, starting a regenerative liquid pump 84, and flushing the system by using the pure water 87 for more than 5 min.
Step 2: the sample pump 82 is turned off, 30mL of the sample to be separated (i.e., coolant) is poured into the sample introduction bottle 81, and the mass m thereof is accurately weighed by an electronic balance0，
And step 3: starting a sample pump 82, feeding samples at the flow rate of about 1.0mL/min, enabling the samples to sequentially pass through a semipermeable membrane separation device 85 and a silver-type ion exchange resin 86, feeding the samples for 20min, putting a sample feeding bottle 81 pipeline into a pure water bottle, 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;
and 4, step 4: accurately weighing the sample injection bottle 81 subjected to sample injection for 20min by using an electronic balance m1Calculating the mass difference between two times of weighing0-m1And the delta m is the sample preparation amount of the loop sample at this time;
and 5: and taking out the silver type ion exchange resin 86 adsorbing the I-131 to complete the separation of the iodine and the isotope thereof.
Step 6: and measuring the I-131 and the isotope activity thereof by using a high-purity germanium spectrometer.
According to the embodiment of the application, the interference reasons of the coolant of the nuclear power plant on the measurement of the iodine and the isotope thereof are determined through sufficient research, the method for separating and collecting the iodine and the isotope thereof is formulated, the nuclides of K-42, N-13, F-18 and the like in the coolant of the primary loop are effectively separated through the semipermeable membrane and the ion exchange column, and the nuclides interfering the measurement of the iodine and the isotope thereof are solved, so that the problem of timely measurement of the iodine and the isotope thereof in the coolant of the primary loop of the nuclear power plant is solved, the purpose of quickly and accurately measuring the iodine and the isotope thereof is achieved, and the detection efficiency and timeliness of the iodine and the isotope are improved.
The present application has been described in detail with reference to the drawings and examples, but the present application is not limited to the above examples, and various changes can be made within the knowledge of those skilled in the art without departing from the spirit of the present application. The prior art can be used for all the matters not described in detail in this application.
Claims (11)
1. A separation system of isotope iodine in nuclear power plant coolant is characterized in that: the system, 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 isotope iodine in the intermediate separator.
2. The separation system of isotope iodine in nuclear power plant coolant of claim 1, characterized in that: the semipermeable membrane separation device comprises: a first semi-permeable membrane, a second semi-permeable membrane and an ionization device;
forming three compartments with the first and second semi-permeable membranes; the three compartments, including: 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 respectively ionizing pure water in the cation regeneration interval and the anion regeneration interval to form cations and anions in the cation regeneration interval and the anion regeneration interval;
the first semi-permeable membrane only allows cations to move from the cation regeneration compartment to the sample compartment; the second semi-permeable 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 separation.
3. The separation system of isotope iodine in nuclear power plant coolant of claim 2, characterized in that: the flow direction of pure water in the cation regeneration compartment and the anion regeneration compartment is opposite to the flow direction of the coolant in the sample compartment.
4. The separation system of isotope iodine in nuclear power plant coolant of claim 2, characterized in that:
the semipermeable membrane separation unit further comprises a first pump for feeding the pure water into the cation regeneration compartment and the anion regeneration compartment;
and/or the presence of a gas in the gas,
the semipermeable membrane separation unit further comprises a second pump for feeding the coolant into the sample compartment.
5. The separation system of isotope iodine in nuclear power plant coolant of claim 1, characterized in that: the ion exchange column is specifically a silver type ion exchange column.
6. The separation system of isotope iodine in nuclear power plant coolant of claim 5, characterized in that: the silver-type ion exchange column comprising: the device comprises a first baffle plate, a second baffle plate and silver type ion exchange resin arranged between the first baffle plate and the second baffle plate;
the first baffle plate is provided with a sample inlet for inputting the intermediate separator;
the second baffle is provided with a sample outlet and is used for outputting waste liquid;
the silver type ion exchange resin is used for adsorbing the isotope iodine.
7. A separation method of isotope iodine in nuclear power plant coolant is characterized in that: a separation system for isotope iodine applied to the nuclear power plant coolant defined in any one of claims 1 to 6; the separation method comprises the following steps:
inputting a coolant into the 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 separated substance, and adsorbing isotope iodine in the intermediate separated substance by the ion exchange column.
8. The method for separating isotope iodine in nuclear power plant coolant as claimed in claim 7, wherein: the input for the coolant to the semipermeable membrane separation unit further comprises:
pre-flushing a separation system of isotope iodine in the nuclear power plant coolant by using pure water;
the input end for inputting the coolant into the semi-permeable membrane separation device further comprises:
and flushing the residual coolant of the isotope iodine separation system in the coolant of the nuclear power plant by using pure water.
9. The method for separating isotope iodine in nuclear power plant coolant as claimed in claim 7, wherein: the input with coolant input semi-permeable membrane separator's input specifically includes:
the coolant was fed to the input of the semipermeable membrane separation unit at a flow rate of 1.0 mL/min.
10. The method for separating isotope iodine in nuclear power plant coolant as claimed in claim 8, wherein: the pre-washing time is 5 minutes; and/or the time of the rinsing is 5 minutes.
11. A method for detecting isotope iodine in a nuclear power plant coolant is characterized by comprising the following steps: a separation system for isotope iodine applied to the nuclear power plant coolant defined in any one of claims 1 to 6; 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 separated substance, and the ion exchange column adsorbs isotope iodine in the intermediate separated substance;
and detecting the isotope iodine adsorbed by the ion exchange column by using a high-purity germanium spectrometer.
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