Multi-nuclide automatic separation and detection system and method

Abstract

The invention provides a multi-nuclide automatic separation and detection system and method, and particularly relates to the technical field of radioactive substance detection. The detection system comprises a cascade separation and regeneration unit, a dynamic regulation and control unit, an online detection unit, an eluent conveying unit and a control system, and the eluent conveying unit is matched with the cascade separation and regeneration unit to separate and purify radionuclide and regenerate resin. The dynamic regulation and control unit is used for controlling a flow path between the eluent conveying unit and the cascade separation regeneration unit and feeding back changes of pressure, temperature and pH value in the flow path in real time, and the online detection unit is used for detecting concentration of nuclides in separation liquid and feeding back monitoring data to the control system. And the control system controls the operation of each functional unit and automatically plans a separation path according to a measurement requirement to form a separation-detection-optimization closed-loop process. The device is suitable for the fields of nuclear facility liquid effluent detection, environmental water radioactivity detection and the like, and has high efficiency, environmental protection property and intelligence.

Description

Technical Field

[0001] This invention relates to the field of radioactive material detection technology, and in particular to an automated separation and detection system and method for multiple nuclides. Background Technology

[0002] The liquid effluent from nuclear power plants typically contains multiple radioactive nuclides. For example, Fe-containing components in a nuclear power plant reactor will simultaneously produce [radioactive nuclides] after neutron activation. 55 Fe and 59 Fe. 55 Fe has a half-life of 2.73 days and emits characteristic X-rays with an energy of 5.9 keV after orbital electron capture. 59 Fe has a half-life of 44.49 days and emits β and γ rays. The β ray energies are 475 keV (51.2%) and 273 keV (48.5%), and the γ ray energies are 1.29 MeV (43%) and 1.09 MeV (57%).

[0003] Ni, as a metallic material, is widely used in various reactor components, and is produced through neutron activation. 63 Ni、 63 Ni is a low-energy pure beta radionuclide with a half-life of 100.1 days and a maximum beta ray energy of 66.95 keV.

[0004] 89 Sr and 90 Sr are all fission products with high radiotoxicity. 89 Sr has a half-life of 50.563 days and undergoes β decay to form a stable nuclide. 89 Y. 90 Sr is an unstable, long-lived radionuclide that can produce radionuclides through beta decay. 90 Y, 90 Y can decay into a stable element. 90 Zr. 89 Sr(Eβmax=1499.3keV), 90 Sr(E βmax =545.9keV) and its daughter bodies 90 Y (Eβmax=2278.5keV) emits only β rays.

[0005] because 89 Sr、 90 Sr、 55 Fe、 63Ni is entirely composed of pure β-nuclides, which cannot be detected by conventional gamma-ray spectroscopy methods and require a complex radiochemical separation process. Currently, the radiochemical separation of these nuclides remains in the era of manual analysis. After on-site sample collection, radiochemical separation is performed in the effluent monitoring laboratory, followed by analysis using a liquid scintillation spectrometer. This method suffers from efficiency bottlenecks, incurs significant human and material costs, and cannot enable timely and effective monitoring and reporting of effluent emission data.

[0006] Therefore, there is a need to provide an automated separation and detection system for multiple nuclides to solve the above problems. Summary of the Invention

[0007] This invention provides an automated multi-nuclein separation and detection system and method to solve the technical problems of low detection efficiency and high manpower and material costs in existing technologies.

[0008] This invention provides an automated multi-nucleoside separation and detection system, comprising: a cascaded separation and regeneration unit, a dynamic control unit, an online detection unit, an eluent delivery unit, and a control system. The cascaded separation and regeneration unit includes a nuclide separation and purification module and a separation liquid collection module. The separation liquid collection module is connected to the nuclide separation and purification module, which is used to separate and purify nuclides in a liquid. The separation liquid collection module is used to collect the separation liquid corresponding to the nuclide. The dynamic control unit includes an intelligent valve switching module and a feedback module. The intelligent valve switching module is used to control the separation of nuclides... The flow path switching of the purification module is described. The feedback module is set on the flow path to provide real-time feedback on changes in pressure, temperature, and pH value in the flow path. The online detection unit is used to detect the concentration of each nuclide in the separation liquid collected by the separation liquid collection module. The eluent delivery unit works with the nuclide separation and purification module to perform nuclide separation and purification. The control system is used to control the operation of the cascade separation regeneration unit, dynamic control unit, online detection unit, and eluent delivery unit, and automatically plans the separation path according to measurement requirements. It also dynamically adjusts the flow rate according to the real-time parameters fed back by the dynamic control unit, forming a closed-loop process of separation-detection-optimization.

[0009] In one embodiment of the present invention, the radionuclide separation and purification module includes a first cation resin column, an anion resin column, a second cation resin column, an iron adsorption resin column, a strontium adsorption resin column, a yttrium adsorption resin column, a nickel adsorption resin column, a temporary storage tank, and a waste liquid collection tank. The first cation resin column is connected to the sample tank. The anion resin column is located downstream of and connected to the first cation resin column. The iron adsorption resin column, the strontium adsorption resin column, the yttrium adsorption resin column, and the nickel adsorption resin column are located in parallel in the downstream branch of the anion resin column. The second cation resin column is located in the connecting branch between the iron adsorption resin column and the anion resin column. The strontium adsorption resin column is connected to the yttrium adsorption resin column. The temporary storage tank is located at the outlet of the yttrium adsorption resin column and is connected to the nickel adsorption resin column. The waste liquid collection tank is connected to each resin column.

[0010] In one embodiment of the present invention, the separation liquid collection module includes an iron separation liquid collection bottle, a strontium separation liquid collection bottle, a yttrium separation liquid collection bottle, and a nickel separation liquid collection bottle, which are respectively connected to the iron adsorption resin column, the strontium adsorption resin column, the yttrium adsorption resin column, and the nickel adsorption resin column via pipelines.

[0011] In one embodiment of the present invention, the intelligent switching valve module includes multiple multi-channel switching valves, multiple dual-flow-path switching valves, and a three-way valve. The multi-channel switching valves are disposed on the connecting pipeline between the radionuclide separation and purification module and the eluent delivery unit. One end of the dual-flow-path switching valve is connected to the multi-channel switching valve, and the other end is connected to the corresponding resin column. The three-way valve is disposed on the connecting pipeline between the radionuclide separation and purification module and the separation liquid collection module.

[0012] In one embodiment of the present invention, the feedback module includes multiple pressure sensors, multiple thermometers and multiple pH meters, which are used to monitor the changes in pressure, temperature and pH value in the flow path, and to feed back real-time pressure, temperature and pH data to the control system to monitor the operating status in real time.

[0013] In one embodiment of the present invention, the eluent delivery unit includes a storage module and a delivery module. The storage module includes reagent bottles for storing nitric acid, hydrochloric acid, ammonium citrate, phosphoric acid, pH adjusting reagent and scintillation solution, respectively. The delivery module includes multiple injection pumps, which are connected to each resin column through pipelines and the intelligent valve switching module.

[0014] In one embodiment of the present invention, the online detection unit includes multiple β detectors, which are respectively connected to the separation liquid collection module to simultaneously measure multiple nuclides and feed the measurement results back to the control system.

[0015] In one embodiment of the present invention, the online detection unit includes a PLC controller, which controls the operation of each functional unit through a built-in program, receives and processes real-time feedback information from each unit.

[0016] In one embodiment of the present invention, the PLC controller employs dynamic decay correction, dynamically adjusting the activity concentration based on the nuclide half-life. The calculation formula is as follows:

[0017]

[0018] In the formula, A is the activity concentration of the target nuclide, in Bq / L; n y n represents the total sample count rate, expressed in cpm. b λ represents the background count rate, in cpm; E represents the instrument's detection efficiency for the target nuclide, in %; V represents the sample volume, in L; R represents the recovery rate of the target nuclide, in %; and λ represents the nuclide decay constant, in min. -1 t represents the dynamically adjusted separation time window, in minutes.

[0019] The present invention also provides a method for detecting multiple nuclides based on the above-mentioned automated separation and detection system for multiple nuclides, comprising:

[0020] Input a radionuclide sample, and the cascaded separation and regeneration unit adsorbs and desorbs the radionuclides in the sample in stages;

[0021] The dynamic control unit feeds back the pressure, temperature and pH information in the flow path to the control system in real time, and the control system monitors the data and handles anomalies in real time.

[0022] After the cascade separation and regeneration unit completes desorption, it generates a separation liquid containing nuclides. The activity concentration of each nuclide is detected by the online detection unit, and the detection data is fed back to the control system.

[0023] The control system dynamically optimizes elution parameters and real-time flow rate data, forming a closed-loop process of separation-detection-optimization.

[0024] The beneficial effects of this invention are as follows: The multi-nucleoside automated separation and detection system proposed in this invention, combining dynamic control algorithm design, cascade separation and regeneration integrated technology, and a separation-detection closed-loop platform, significantly improves the efficiency and intelligence level of nuclide separation. By monitoring the flow path status in real time, the separation path and parameters are dynamically optimized; a cascade adsorption-desorption process is used to achieve step-by-step separation of multiple nuclides and online resin regeneration; the online detection unit monitors the separation effect in real time and provides feedback for adjustment, forming a closed-loop control. This invention is applicable to fields such as the detection of liquid effluents from nuclear facilities and the detection of radioactivity in environmental water, combining high efficiency, environmental friendliness, and intelligence. Attached Figure Description

[0025] The accompanying drawings, which are incorporated in and form part of this specification, illustrate embodiments consistent with this application and, together with the description, serve to explain the principles of this application. It is obvious that the drawings described below are merely some embodiments of this application, and those skilled in the art can obtain other drawings based on these drawings without any inventive effort.

[0026] In the attached diagram:

[0027] Figure 1 This is a schematic diagram of the logical connection of an automated multi-nuclein separation and detection system provided in an embodiment of the present invention;

[0028] Figure 2 This is a schematic diagram showing the connection of each unit in an embodiment of the multi-nucleoside automatic separation and detection system provided by the present invention.

[0029] Figure 3 This is a schematic diagram showing the connection of each component in the cascade separation and regeneration unit of the multi-nucleoside automatic separation and detection system provided in one embodiment of the present invention;

[0030] Figure 4 This is a schematic diagram showing the connection between the eluent delivery unit, the dynamic control unit, and the cascade separation and regeneration unit of the multi-nucleoside automatic separation and detection system provided in one embodiment of the present invention.

[0031] Figure 5 This is a flowchart of the detection steps of an automated multi-nucleoside separation and detection system provided in one embodiment of the present invention.

[0032] The attached figures are labeled as follows:

[0033] 100. Cascaded Separation and Regeneration Unit; 110. Radionuclide Separation and Purification Module; 111. First Cation Resin Column; 112. Anion Resin Column; 113. Second Cation Resin Column; 114. Iron Adsorption Resin Column; 115. Strontium Adsorption Resin Column; 116. Yttrium Adsorption Resin Column; 117. Nickel Adsorption Resin Column; 118. Temporary Storage Tank; 119. Waste Liquid Collection Tank; 120. Separation Liquid Collection Module; 121. Iron Separation Liquid Collection Bottle; 122. Strontium Separation Liquid Collection Bottle; 123. Yttrium Separation Liquid Collection bottle; 124, Nickel separation solution collection bottle; 200, Dynamic control unit; 210, Intelligent valve switching module; 211, Multi-channel switching valve; 212, Dual-flow path switching valve; 213, Three-way valve; 220, Feedback module; 221, Pressure sensor; 222, Thermometer; 223, pH meter; 300, Online detection unit; 400, Eluent delivery unit; 410, Liquid storage module; 411, Reagent bottle; 420, Delivery module; 421, Injection pump; 500, Control system. Detailed Implementation

[0034] The following specific examples illustrate the implementation of the present invention. Those skilled in the art can easily understand other advantages and effects of the present invention from the content disclosed in this specification. The present invention can also be implemented or applied through other different specific embodiments. Various details in this specification can also be modified or changed based on different viewpoints and applications without departing from the spirit of the present invention. In the absence of conflict, the following embodiments and features in the embodiments can be combined with each other.

[0035] It should be noted that the illustrations provided in the following embodiments are only schematic representations of the basic concept of the present invention. The drawings only show the components related to the present invention and are not drawn according to the actual number, shape and size of the components in the actual implementation. In the actual implementation, the form, quantity and proportion of each component can be arbitrarily changed, and the layout of the components may also be more complex.

[0036] In the following description, numerous details are explored to provide a more thorough explanation of embodiments of the invention. However, it will be apparent to those skilled in the art that embodiments of the invention may be practiced without these specific details. In other embodiments, well-known structures and devices are shown in block diagram form rather than in detail to avoid obscuring embodiments of the invention.

[0037] Please see Figure 1 This invention provides an automated multi-nucleoside separation and detection system for automatically separating iron (Fe), nickel (Ni), strontium (Sr), and yttrium (Y) nuclides from liquids and then automatically measuring them. The system includes a cascaded separation and regeneration unit 100, a dynamic control unit 200, an online detection unit 300, an eluent delivery unit 400, and a control system 500. The eluent delivery unit 400 is used to deliver pretreatment solution, desorption solution, and regeneration solution to the cascade separation and regeneration unit 100, which works in conjunction with the cascade separation and regeneration unit 100 to separate and purify radionuclides and regenerate resin. The dynamic control unit 200 is used to control the flow path between the eluent delivery unit 400 and the cascade separation and regeneration unit 100, and to provide real-time feedback on changes in pressure, temperature, and pH in the flow path. The online detection unit 300 is used to detect the concentration of each nuclide in the separation solution of the cascade separation and regeneration unit 100 and to feed back the monitoring data to the control system 500. The control system 500 controls the operation of the cascade separation and regeneration unit 100, the dynamic control unit 200, the online detection unit 300, and the eluent delivery unit 400, and automatically plans the separation path according to measurement requirements. It also dynamically adjusts the flow rate according to the real-time parameters fed back by the dynamic control unit, forming a closed-loop process of separation-detection-optimization.

[0038] Please see Figure 2 and Figure 3The cascaded separation and regeneration unit 100 includes a radionuclide separation and purification module 110 and a separation liquid collection module 120. The radionuclide separation and purification module 110 is used to separate and purify multiple radionuclides in the liquid. The separation liquid collection module 120 is connected to the radionuclide separation and purification module 110 and is used to collect the separation liquid containing each radionuclide. The radionuclide separation and purification module 110 includes multiple resin columns, the type and number of which are related to the types of radionuclides to be separated. In one embodiment, if the liquid to be separated contains radionuclides such as Fe, Ni, and Sr, then the radionuclide separation and purification module 110 includes a first cation resin column 111, an anion resin column 112, a second cation resin column 113, an iron adsorption resin column 114, a strontium adsorption resin column 115, a yttrium adsorption resin column 116, a nickel adsorption resin column 117, a temporary storage tank 118, and a waste liquid collection tank 119. The first cation resin column 111 is connected to a sample tank (not shown in the figure) containing liquid effluent and the waste liquid collection tank 119 via pipelines. The liquid effluent flows from the sample container into the first cation exchange resin column 111. Because the cation exchange resin column contains a large number of anionic groups, such as sulfonic acid groups (-SO3),... - ), carboxyl group (-COO) -The liquid contains radioactive nuclides, which exist as positively charged cations. When the liquid effluent flows through the first cation exchange resin column 111, Fe, Ni, Sr, and other ions inside are adsorbed onto the first cation exchange resin column 111 through electrostatic adsorption or ion exchange reaction. The liquid effluent is then discharged into the waste liquid collection tank 119. The anion exchange resin column 112 is located downstream of and connected to the first cation exchange resin column 111. When desorption occurs on the first cation exchange resin column 111, the desorbed liquid is transported to the first cation exchange resin column 111 by the eluent delivery unit. After desorption, it enters the anion exchange resin column 112, where Fe ions are adsorbed onto the anion exchange resin column 112. The desorbed liquid then flows downstream. Iron adsorption resin column 114, strontium adsorption resin column 115, yttrium adsorption resin column 116, and nickel adsorption resin column 117 are arranged in parallel in the downstream branch of anion exchange resin column 112. A second cation exchange resin column 113 is located in the connecting branch between iron adsorption resin column 114 and anion exchange resin column 112. The second cation exchange resin column 113 can further purify iron ions in the desorbate from anion exchange resin column 112. Strontium adsorption resin column 115 and yttrium adsorption resin column 116 are connected by a pipeline. A temporary storage tank 118 is located at the outlet of yttrium adsorption resin column 116 and is connected to nickel adsorption resin column 117 via a pipeline. Waste liquid collection tanks 119 are connected to each resin column. The separation liquid collection module 120 includes multiple separation liquid collection bottles, the number of which is related to the number of nuclides to be separated. In this embodiment, the separation liquid collection module 120 includes an iron separation liquid collection bottle 121, a strontium separation liquid collection bottle 122, a yttrium separation liquid collection bottle 123, and a nickel separation liquid collection bottle 124. The iron separation liquid collection bottle 121, the strontium separation liquid collection bottle 122, the yttrium separation liquid collection bottle 123, and the nickel separation liquid collection bottle 124 are respectively connected to the iron adsorption resin column 114, the strontium adsorption resin column 115, the yttrium adsorption resin column 116, and the nickel adsorption resin column 117.

[0039] Please see Figure 2 and Figure 4The dynamic control unit 200 includes an intelligent valve switching module 210 and a feedback module 220. The intelligent valve switching module 210 includes several switching valves, which are installed on various pipelines of the cascade separation and regeneration unit 100, allowing for several flow path combinations. The feedback module 220 can provide real-time feedback on changes in pressure, temperature, and pH value in the flow path. In one embodiment, the intelligent valve switching module 210 includes multiple multi-channel switching valves 211, multiple dual-flow-path switching valves 212, and multiple three-way valves 213. The multiple multi-channel switching valves 211 are respectively connected to each resin column of the cascade separation and regeneration unit 100 and the eluent delivery unit 400 through pipelines. The number of multi-channel switching valves 211 is related to the type of reagent in the eluent delivery unit 400. The multiple dual-flow-path switching valves 212 respectively connect each resin column of the cascade separation and regeneration unit 100 to the multi-channel switching valves 211, and the number of dual-flow-path switching valves 212 is consistent with the number of resin columns. Three-way valves 213 are installed on the connecting pipeline between the radionuclide separation and purification module 110 and the separation liquid collection module 120. Specifically, multiple three-way valves 213 are respectively installed on the drain pipelines of the iron adsorption resin column 114, strontium adsorption resin column 115, yttrium adsorption resin column 116, and nickel adsorption resin column 117. One end of the three-way valve 213 is connected to the resin column, the other end is connected to the separation liquid collection bottle corresponding to the resin column, and the remaining end is connected to the waste liquid collection tank 119. In this embodiment, the feedback module 220 includes fourteen pressure sensors 221, eight thermometers 222, and nine pH meters 223. The fourteen pressure sensors 221 are respectively installed at the inlet and outlet ends of the seven resin columns of the cascade separation and regeneration unit 100 to monitor the pressure changes in the pipeline in real time and feed the data back to the control system 500 to adjust the flow rate. One pH meter 223 is installed in the sample container, another pH meter 223 is installed in the temporary storage tank 118 at the liquid inlet of the nickel adsorption resin column 117, and the remaining seven pH meters 223 are respectively installed at the liquid inlet of the seven resin columns of the cascade separation and regeneration unit 100. One thermometer 222 is installed in the temporary storage tank 118 at the liquid inlet of the nickel adsorption resin column 117, and the seven thermometers 222 are respectively installed at the liquid outlet of the seven resin columns. These are used to feed back real-time pressure, temperature and pH data to the control system 500, so that the control system 500 can monitor the operating status in real time and provide timely feedback when abnormalities occur.

[0040] Please see Figure 2 and Figure 4The eluent delivery unit 400 includes a storage module 410 and a delivery module 420. The storage module 410 includes multiple reagent bottles 411 for storing nitric acid, hydrochloric acid, phosphoric acid, ammonium citrate, pH adjustment reagent, and scintillation fluid. The nitric acid is available in two concentrations: 0.05-0.1M and 6-8M. The hydrochloric acid is available in two concentrations: 0.05M-0.1M and 4-6M. The ammonium citrate solution has a concentration of 1M-3M, and the phosphoric acid solution has a concentration of 0.5M-1M. Nitric acid can be used as a pretreatment solution to pretreat each resin column. The concentration of nitric acid used in resin column pretreatment depends on the type of resin column. For example, the pretreatment solution for cation exchange resin columns is 0.1M nitric acid, the pretreatment solution for nickel adsorption resin column 117 is 1M ammonium citrate, and the pretreatment solution for anion exchange resin columns 112, iron adsorption resin column 114, strontium adsorption resin column 115, and yttrium adsorption resin column 116 is 8M nitric acid. Nitric acid, hydrochloric acid, and phosphoric acid can be used as eluents; the choice depends on the type of resin column. Ammonia can be used as a pH adjusting agent. Nitric acid and hydrochloric acid of different concentrations should be stored in separate reagent bottles (411). Figure 2 The reagent bottle 411 is shown only as an example; the number of reagent bottles in the figure does not represent the actual number used in practice. The number of reagent bottles 411 can be set according to actual needs. The delivery module 420 includes multiple syringe pumps 421. Under the control of the control system 500, the multiple syringe pumps 421 deliver the solutions from the multiple reagent bottles 411 to the corresponding resin columns of the cascade separation and regeneration unit 100 according to instructions, so as to cooperate with the cascade separation and regeneration unit 100 to complete the separation and purification of radionuclides in the liquid. Here, the number of syringe pumps 421 is consistent with the number of reagent bottles 411.

[0041] Please see Figure 1 and Figure 2 The online detection unit 300 includes multiple β detectors 310, the number of which corresponds to the number of nuclides to be detected. The online detection unit 300 integrates a β array detector, which can automatically monitor the concentration of each nuclide in the separation solution and simultaneously feed the detection data back to the control system 500. In one embodiment, the online detection unit 300 includes four β detectors, employing both β counting and Cherenkov counting modes to measure low-energy β nuclides (…). 55 Fe、 63 Ni) and high-energy β nuclides ( 89 Sr、 90 The measurement data is transmitted to the control system 500, and the detection data is uploaded to the data recording platform in real time to generate an encrypted and tamper-proof separation process traceability record.

[0042] Please see Figure 1The control system 500 includes a PLC controller and a built-in program. The PLC controller runs dynamic optimization algorithms (PID control, decay correction model, dynamic flow path control algorithm), controls the operation of each functional unit through the built-in program, and receives and processes real-time feedback information from each unit. It automatically plans the separation path according to measurement requirements and dynamically adjusts the flow rate based on real-time parameters fed back from the dynamic control unit, forming a closed-loop process of separation-detection-optimization.

[0043] Furthermore, the built-in dynamic optimization algorithm includes: a feedback control model based on detection data to adjust the flow rate in real time;

[0044] The decay correction module dynamically adjusts the activity concentration based on the nuclide's half-life. The calculation formula is as follows:

[0045]

[0046] Where A is the activity concentration of the target nuclide, in Bq / L; n y n represents the total sample count rate, expressed in cpm. b λ represents the background count rate (cpm); E represents the instrument's detection efficiency for the target nuclide (%); V represents the sample volume (L); R represents the recovery rate of the target nuclide (%); and λ represents the nuclide decay constant (min). -1 t represents the dynamically adjusted separation time window, in minutes.

[0047] The control process of the control system 500 for each functional unit is as follows: The control system 500 controls the eluent delivery unit 400 to deliver pretreatment liquid to the cascade separation and regeneration unit 100. First, the first cation resin column 111, the anion resin column 112, the second cation resin column 113, the iron adsorption resin column 114, the strontium adsorption resin column 115, the yttrium adsorption resin column 116, and the nickel adsorption resin column 117 are pretreated to reach the required pH. Then, the sample (liquid effluent) is injected into the first cation resin column 111. The cations (radioactive elements) in the sample are adsorbed on the first cation resin column 111, and the effluent is discharged to the waste liquid collection tank 119. The desorption process is then performed: the cation resin desorption solution is first injected into the first cation resin column 111 through the eluent delivery unit 400. The effluent passes sequentially through the anion resin column 112, the strontium adsorption resin column 115, and the yttrium adsorption resin column 116 and is then collected in the temporary storage tank 118. The pH value of the effluent in the temporary storage tank 118 is adjusted to 8-9 using ammonia water, and then injected into the nickel adsorption resin column 117. After being adsorbed by the nickel adsorption resin column 117, it is discharged into the waste liquid collection tank 119. Then, the desorption solution of the anion exchange resin column 112 is injected into the anion exchange resin column 112, and the effluent passes through the second cation exchange resin column 113 and is discharged into the waste liquid collection tank 119; the desorption solution of the cation exchange resin is then injected into the second cation exchange resin column 113, and the effluent passes through the iron adsorption resin column 114 and is discharged into the waste liquid collection tank 119; the desorption solutions of the iron adsorption resin, strontium adsorption resin, yttrium adsorption resin, and nickel adsorption resin are injected into the iron adsorption resin column 114, strontium adsorption resin column 115, yttrium adsorption resin column 116, and nickel adsorption resin column 117, respectively, to obtain separation solutions containing Fe, Ni, Sr, and Y, which are collected in the corresponding separation solution collection bottles. Finally, the regenerated solution is injected into the first cation resin column 111, the anion resin column 112, the second cation resin column 113, the iron adsorption resin column 114, the strontium adsorption resin column 115, the yttrium adsorption resin column 116, and the nickel adsorption resin column 117 respectively to achieve resin regeneration.

[0048] The Fe, Ni, Y, and S-containing separation liquid in the separation liquid collection bottle is injected into the detector of the online detection unit 300. After the measurement is completed by the β array detector, the result is output to the control system 500. After processing by the preset program, the raw data and the processing result are uploaded to the data recording platform.

[0049] In one embodiment, the control system 500 can automatically plan the separation path according to the monitoring requirements of the sample. If the sample only needs to measure Fe nuclides, the desorption solution of the anion exchange resin column 112 does not pass through the strontium adsorption resin column 115, the yttrium adsorption resin column 116 and the nickel adsorption resin column 117.

[0050] Please see Figures 1 to 5The present invention also provides a detection method using the above-mentioned automated separation and detection system, comprising the following steps:

[0051] S1. Input the nuclide sample, and the cascade separation and regeneration unit 100 adsorbs and desorbs the nuclide in the sample step by step.

[0052] S2. The dynamic control unit 200 feeds back the pressure, temperature and pH information in the flow path to the control system 500 in real time. The control system 500 monitors the data in real time and handles anomalies.

[0053] S3. After the cascade separation and regeneration unit 100 completes desorption, it generates a separation liquid containing nuclides. The activity concentration of each nuclide is detected by the online detection unit 300, and the detection data is fed back to the control system 500.

[0054] S4. The control system 500 dynamically optimizes the elution parameters and real-time flow rate data to form a closed-loop process of separation-detection-optimization.

[0055] Specifically, before executing step S1, each resin column of the cascade separation and regeneration unit 100 is pretreated to achieve the required pH. For example, the first cation exchange resin column 111 and the second cation exchange resin column 113 use 0.1M HNO3, 20 mL, at a flow rate of 4 mL / min; the nickel adsorption resin column 117 uses 1M ammonium citrate, 20 mL, at a flow rate of 4 mL / min; the anion exchange resin column 112, the iron adsorption resin column 114, the strontium adsorption resin column 115, and the yttrium adsorption resin column 116 use 8M HNO3, 20 mL, at a flow rate of 4 mL / min. The pretreatment solution for this pretreatment process is injected into the corresponding reagent bottle via the syringe pump of the eluent delivery unit 400.

[0056] The processing procedure of the cascaded separation and regeneration unit 100 in step S1 is as follows:

[0057] Input of radionuclide sample: After the liquid effluent is adjusted to pH 2.0±0.1 by an online pH meter, it is pumped into the first cation exchange resin column 111 at a rate of 4 mL / min by a syringe pump.

[0058] Nuclide separation process:

[0059] 55 Fe separation:

[0060] (1) Use a syringe pump to draw 8M HNO3 (30mL) to rinse the first cation exchange resin column 111, Fe 3+ FeCl4 - The eluent enters the anion exchange resin column 112, and after passing through the strontium adsorption resin column 115 and the yttrium adsorption resin column 116, it is collected and the pH is adjusted to 8-9 with ammonia.

[0061] (2) Use a syringe pump to draw 4-6M HCl (40mL) to wash the anion exchange resin column 112 and remove impurity ions;

[0062] (3) Use a syringe pump to draw 0.05-0.1M HCl (30mL) to elute Fe. 3+ To the second cation exchange resin column 113;

[0063] (4) Use a syringe pump to draw 6-8M HNO3 (30mL) to elute Fe. 3+ To the iron adsorption resin column 114;

[0064] (5) Use a syringe pump to draw 0.5M-1M HPO4 (10mL) to elute Fe from the iron adsorption resin column 114. 3+ To the iron separation liquid collection bottle 121.

[0065] 63 Ni separation:

[0066] (1) The eluent (pH 8.5, 20 mL) after pH adjustment with ammonia in step 1 was drawn by a syringe pump and passed through a nickel adsorption resin column 117. 2+ Entering the nickel column;

[0067] (2) Use a syringe pump to draw 10 mL of 3 M HCl to elute the Ni in column 117 of the nickel adsorption resin. 2+ Transfer to nickel separation solution collection bottle 122.

[0068] Sr isotope separation:

[0069] (1) Use a syringe pump to draw 0.1M HNO3 (10mL) to elute the strontium adsorption resin column 115. 89 Sr to Strontium separation solution collection bottle 123.

[0070] (2) Use a syringe pump to draw 0.1M HCl (10mL) to elute the yttrium adsorption resin column 116. 90 Sr( 90 Y), to yttrium separation solution collection bottle 124.

[0071] In step S2, during the execution of step S1, the intelligent valve switching module 210 of the dynamic control unit 200 works with the eluent delivery unit 400 to control the opening and closing of each pipeline. The feedback module 220 monitors the changes in pressure, temperature and pH value in the flow path in real time and feeds them back to the control system 500. If the real-time monitoring data is abnormal, the control system 500 will handle it in a timely manner.

[0072] Step S3, the detection step, involves the generation of radionuclide-containing separation solutions after desorption from each resin column in the cascade separation and regeneration unit 100. These solutions are collected in iron separation solution collection bottles 121, nickel separation solution collection bottles 122, strontium separation solution collection bottles 123, and yttrium separation solution collection bottles 124. These solutions are then detected by the online detection unit 300, specifically: the iron and nickel separation solutions are detected using the β-counting detection unit of the β-detector 310, while the strontium and yttrium separation solutions are detected using the Cherenkov detection unit of the β-detector 310. The detection data is then fed back to the control system 500.

[0073] Step S4 involves the control system 500 processing various parameters and detection data through its built-in program to form a closed-loop process of separation-detection-optimization. It should be noted that the built-in program of the control system 500 can be a conventional program in this field, and will not be detailed here.

[0074] Those skilled in the art should understand that the above steps S1-S4 are only set up for the convenience of describing the detection process and do not indicate the order of steps.

[0075] The automated multi-nucleoside separation and detection system provided by this invention, combining dynamic control algorithm design, cascaded separation and regeneration integrated technology, and a separation-detection closed-loop platform, significantly improves nuclide separation efficiency and intelligence. It dynamically optimizes the separation path and parameters by real-time monitoring of the flow path status; employs a cascaded adsorption-desorption process to achieve step-by-step separation of multiple nuclides and online resin regeneration; and an online detection unit monitors the separation effect in real time and provides feedback for adjustment, forming a closed-loop control. This invention is applicable to fields such as the detection of liquid effluents from nuclear facilities and the detection of radioactivity in environmental water, combining high efficiency, environmental friendliness, and intelligence.

[0076] The above embodiments are merely illustrative of the principles and effects of the present invention and are not intended to limit the invention. Any person skilled in the art can modify or alter the above embodiments without departing from the spirit and scope of the present invention. Therefore, all equivalent modifications or alterations made by those skilled in the art without departing from the spirit and technical concept disclosed in the present invention should still be covered by the claims of the present invention.

Claims

1. An automated multi-nucleoside separation and detection system, characterized in that, include: A cascaded separation and regeneration unit includes a radionuclide separation and purification module and a separation liquid collection module. The separation liquid collection module is connected to the radionuclide separation and purification module. The radionuclide separation and purification module is used to separate and purify radionuclides in a liquid, and the separation liquid collection module is used to collect the separation liquid corresponding to the radionuclide. The dynamic control unit includes an intelligent valve switching module and a feedback module. The intelligent valve switching module is used to control the flow path switching of the radionuclide separation and purification module. The feedback module is set on the flow path to provide real-time feedback on changes in pressure, temperature, and pH value in the flow path. An online detection unit is used to detect the concentration of each nuclide in the separation liquid collected by the separation liquid collection module; The eluent delivery unit works in conjunction with the radionuclide separation and purification module to perform radionuclide separation and purification. The control system is used to control the operation of the cascaded separation and regeneration unit, dynamic control unit, online detection unit and eluent delivery unit, and automatically plan the separation path according to measurement requirements, and dynamically adjust the flow rate according to the real-time parameters fed back by the dynamic control unit, forming a closed-loop process of separation-detection-optimization.

2. The automated multi-nucleoside separation and detection system according to claim 1, characterized in that, The radionuclide separation and purification module includes a first cation resin column, an anion resin column, a second cation resin column, an iron adsorption resin column, a strontium adsorption resin column, a yttrium adsorption resin column, a nickel adsorption resin column, a temporary storage tank, and a waste liquid collection tank. The first cation resin column is connected to the sample tank. The anion resin column is located downstream of and connected to the first cation resin column. The iron adsorption resin column, the strontium adsorption resin column, the yttrium adsorption resin column, and the nickel adsorption resin column are located in parallel on the downstream branch of the anion resin column. The second cation resin column is located on the connecting branch between the iron adsorption resin column and the anion resin column. The strontium adsorption resin column is connected to the yttrium adsorption resin column. The temporary storage tank is located at the outlet of the yttrium adsorption resin column and is connected to the nickel adsorption resin column. The waste liquid collection tank is connected to each resin column.

3. The automated multi-nucleoside separation and detection system according to claim 2, characterized in that, The separation liquid collection module includes an iron separation liquid collection bottle, a strontium separation liquid collection bottle, a yttrium separation liquid collection bottle, and a nickel separation liquid collection bottle, which are respectively connected to the iron adsorption resin column, the strontium adsorption resin column, the yttrium adsorption resin column, and the nickel adsorption resin column via pipelines.

4. The automated multi-nucleoside separation and detection system according to claim 1, characterized in that, The intelligent valve switching module includes multiple multi-channel switching valves, multiple dual-flow-path switching valves, and a three-way valve. The multi-channel switching valves are installed on the connecting pipeline between the radionuclide separation and purification module and the eluent delivery unit. One end of the dual-flow-path switching valve is connected to the multi-channel switching valve, and the other end is connected to the corresponding resin column. The three-way valve is installed on the connecting pipeline between the radionuclide separation and purification module and the separation liquid collection module.

5. The automated multi-nucleoside separation and detection system according to claim 4, characterized in that, The feedback module includes multiple pressure sensors, multiple thermometers, and multiple pH meters, which are used to monitor the changes in pressure, temperature, and pH in the flow path, and to feed back real-time pressure, temperature, and pH data to the control system for real-time monitoring of the operating status.

6. The automated multi-nucleoside separation and detection system according to claim 1, characterized in that, The eluent delivery unit includes a storage module and a delivery module. The storage module includes reagent bottles for storing nitric acid, hydrochloric acid, ammonium citrate, phosphoric acid, pH adjusting reagent, and scintillation solution, respectively. The delivery module includes multiple injection pumps, which are connected to each resin column via pipelines and the intelligent valve switching module.

7. The automated multi-nucleoside separation and detection system according to claim 1, characterized in that, The online detection unit includes multiple β detectors, each of which is connected to the separation liquid collection module to simultaneously measure multiple nuclides and feed the measurement results back to the control system.

8. The automated multi-nucleoside separation and detection system according to claim 1, characterized in that, The online detection unit includes a PLC controller, which controls the operation of each functional unit through a built-in program, receives and processes real-time feedback information from each unit.

9. The automated multi-nucleoside separation and detection system according to claim 8, characterized in that, The PLC controller employs dynamic decay correction, dynamically adjusting the activity concentration based on the nuclide's half-life. The calculation formula is as follows: In the formula, A is the activity concentration of the target nuclide, in Bq / L; n y n represents the total sample count rate, expressed in cpm. b The background count rate is expressed in cpm; E is the instrument's detection efficiency for the target nuclide, %; V is the sample volume, in L; and R is the recovery rate of the target nuclide, %; λ is the nuclide decay constant, in min. -1 ; t is the dynamically adjusted separation time window, in minutes.

10. A method for detecting multiple nuclides based on any one of the automated separation and detection systems for multiple nuclides according to claims 1 to 9, characterized in that, Includes the following steps: Input a radionuclide sample, and the cascaded separation and regeneration unit adsorbs and desorbs the radionuclides in the sample in stages; The dynamic control unit feeds back the pressure, temperature and pH information in the flow path to the control system in real time, and the control system monitors the data and handles anomalies in real time. After the cascade separation and regeneration unit completes desorption, it generates a separation liquid containing nuclides. The activity concentration of each nuclide is detected by the online detection unit, and the detection data is fed back to the control system. The control system dynamically optimizes elution parameters and real-time flow rate data, forming a closed-loop process of separation-detection-optimization.

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