Device and method for preparing 239Np tracer agent through double-column circulation

Abstract

The invention relates to a device and a method for preparing a < 239 > Np tracer through double-column circulation, belongs to the technical field of separation and preparation of actinide isotopes, and solves the technical problems of low parent and daughter purity and unstable recovery rate in preparation of the < 239 > Np tracer. The device comprises a temperature controller, a radiation shield, a liquid storage tank unit, a color layer separation unit, a waste liquid collector, a product collector, a valve and a delivery pump. Liquid in the liquid storage tank unit enters the color layer separation unit through the conveying pump, and liquid flowing out of the color layer separation unit enters the waste liquid collector or the product collector. And the color layer separation unit comprises a TODGA color layer adsorption column and an LN or P204 or P507 color layer adsorption column. The method comprises the following steps: preparing feed liquid, washing liquid, leacheate and a color layer adsorption column before separation; and neptunium adsorption, washing and leaching. The method is used for preparing the 239Np tracer agent.

Description

Technical Field

[0001] The present invention belongs to the technical field of separation and preparation of actinide isotopes, and specifically relates to a double-column circulation preparation method. 239 Np tracer device and method. Background Art

[0002] 239 Np has a half-life of 2.35 days and is a short-lived γ-radionuclide. It is often used to identify long-lived α-radionuclides in the actinide series in environmental samples. 237 Np (half-life 2.14×10 6 It can be produced in two ways: the first method uses 238 U neutron activation reaction produces 239 U (half-life 23.5 minutes), 239 U will soon be available through beta - Decay Generation 239 Np, this method not only requires the use of expensive neutron source irradiation equipment, but also requires the solution of a large number of target nuclei. 238 U, fission products and 239 The separation of Np is not commonly used in laboratories. The second method is the parent nuclide 243 Am (half-life 7370 years) generates daughters through its own α decay 239 Np. Due to the parent nuclide 243 The half-life of Am is much longer than that of daughter nuclides 239 Np, and therefore undergoes a certain daughter nucleus half-life, 243 Am can generate a certain activity 239 Np can be separated and extracted from the mother nuclide. This method is a "cow milking" preparation method and is also commonly used in laboratories. 239 Np tracer preparation method.

[0003] Extraction chromatography is often used because it combines the high selectivity of solvent extraction with the high efficiency of chromatographic separation. 239 Preparation of Np tracer. 239 Npfrom 243 Am. J Radioanal Nucl Chem. 2005, 266 (1): 71-74) reported that based on the principle of ferrous aminosulfonate reduction, the tetravalent neptunium and trivalent americium were separated by using Aliquat-336 silica gel column. However, the neptunium was not only contaminated with 0.5% americium, but also the recovered 243The Am mother liquor contains impurities such as Fe ions introduced during the reduction process, and additional steps are required to remove these interfering substances before the next step can be carried out. 239 Np preparation is very inconvenient. Patent (ZL 201310626323.7 Shi Yanmei et al. 239 The method reported in the rapid preparation of Np tracer is relatively simple, but the recovered 243 Am mother liquid medium and next 239 The medium required for the column of Np preparation is inconsistent, and lengthy transfer steps such as evaporation, conversion, and re-dissolution are required before it can be used for the next preparation, which inevitably causes 243 The loss of Am, and this method does not control the valence state of neptunium, making it difficult to ensure 239 Stability and reproducibility of Np tracer recoveries.

[0004] because 239 Np has a short half-life, and each preparation 239 The Np tracer decays quickly. Therefore, frequent “milking” is required to meet the needs of routine, multi-batch sample preparation. 237 This requires that the process implementation of both the first preparation and the subsequent multiple preparations should be simpler and easier, and both the parent and daughter products should have sufficiently high purity and recovery rate. Obviously, the above method cannot meet the current technical needs well. Summary of the invention

[0005] To overcome 239 The preparation of Np tracer has the disadvantages of low purity of parent and daughter and unstable recovery rate. The present invention proposes a double column circulation preparation method. 239 Np tracer device and method.

[0006] The technical solution adopted by the present invention to solve the technical problem is:

[0007] A double column circulation preparation 239 The device for Np tracer includes a temperature controller, a radiation shield, a liquid storage tank unit, a chromatography separation unit, a waste liquid collector, a product collector, a valve, a delivery pump and a pipeline;

[0008] The temperature controller is a constant temperature electric heating jacket or electric heating belt or water bath, which is placed outside the radioactive solution storage tank containing americium and neptunium.

[0009] The radiation shielding body is lead brick or lead-containing material and is placed outside the temperature controller.

[0010] The above-mentioned liquid storage tank unit, chromatographic separation unit, waste liquid collector, valve and product collector are connected by pipelines;

[0011] The above-mentioned liquid storage tank unit includes a feed liquid storage tank, a washing liquid storage tank, a first-stage eluent storage tank, a second-stage eluent storage tank and a third-stage eluent storage tank;

[0012] The above-mentioned chromatographic separation unit includes a TODGA chromatographic adsorption column and a LN or P 204 or P 507 Chromatographic adsorption column;

[0013] The bottom of the liquid storage tank is connected to the inlet of the delivery pump through a pipeline and a valve; the outlets of the washing liquid storage tank, the first-stage eluent storage tank, the second-stage eluent storage tank and the third-stage eluent storage tank are connected to the inlet of the delivery pump through a valve;

[0014] The outlet of the delivery pump is connected to the TODGA chromatography column and LN or P 204 or P 507 The inlet connection of the chromatography adsorption column;

[0015] The outlet of the TODGA chromatography column is connected to the waste liquid collector, LN or P through a valve. 204 or P 507 The inlet of the chromatography adsorption column is connected to the product collector;

[0016] LN or P above 204 or P 507 The discharge port of the chromatography adsorption column is connected to the waste liquid collector and the storage tank containing the radioactive solution of americium and neptunium through valves respectively;

[0017] The above pipelines use silicone tubes; the valves are solenoid valves; and the delivery pumps are peristaltic pumps. In this way, the solenoid valves and peristaltic pumps can be controlled by a microcomputer to achieve automatic control of the separation process, reducing the impact of radioactive nuclides radiation and toxicity on the human body during separation. The peristaltic pump uses a hose to squeeze the liquid for separation, and controls the flow rate and velocity of the liquid through the rotation speed of the peristaltic pump.

[0018] A double column circulation preparation 239 The method of Np tracer comprises the following steps:

[0019] Step 1: Preparation before separation

[0020] Add 100 mg of sodium nitrite to the radioactive solution containing americium and neptunium, keep the temperature at 70-100 degrees for 15 minutes, and cool to form a feed solution before separation;

[0021] Dissolving the acid in water respectively to form an aqueous washing solution and an aqueous eluent;

[0022] TODGA, LN or P 204 or P 507 The resins are respectively loaded into chromatography columns;

[0023] Step 2: Adsorption of Americium and Neptunium

[0024] The aqueous radioactive solution containing americium and neptunium prepared in step 1 is passed through a TODGA chromatography adsorption column to adsorb americium and neptunium, and the effluent is collected as waste liquid;

[0025] Step 3: Washing

[0026] The washing liquid is washed through the TODGA chromatography adsorption column, and the effluent is collected as waste liquid;

[0027] Step 4: Rinse

[0028] The first-stage eluent is passed through a TODGA chromatography column to desorb neptunium; the effluent, i.e. the radioactive solution of neptunium, is collected in a product collector;

[0029] The second stage eluent passes through the TODGA chromatography adsorption column and LN or P 204 or P 507 The chromatographic adsorption column is used to desorb and re-adsorb americium, and the effluent is collected as waste liquid;

[0030] The first stage eluent is LN or P 204 or P 507 The chromatographic adsorption column is washed and the effluent is collected as waste liquid;

[0031] Washing liquid is passed through LN or P 204 or P 507 The chromatographic adsorption column is used to desorb americium, and the effluent, i.e., the radioactive solution of americium, is collected in a storage tank of the radioactive solution of americium and neptunium;

[0032] Step 5: Regeneration

[0033] The third-stage eluent passes through the TODGA chromatography adsorption column, and the effluent is collected as waste liquid;

[0034] The second stage eluent is LN or P 204 or P 507 The pipeline between the chromatography adsorption column and the TODGA chromatography adsorption column, the effluent is collected as waste liquid;

[0035] The second stage eluent is LN or P 204 or P 507 Chromatographic adsorption column, the effluent is collected as waste liquid;

[0036] The washing liquid passes through the TODGA chromatography adsorption column, and the effluent is collected as waste liquid;

[0037] Step 6: Recycling

[0038] After the americium solution in the americium-neptunium radioactive solution storage tank is left for 7 to 8 days, sufficient new 239Np, repeat steps 1 to 5 to enter the next preparation process, and repeat the preparation in this way. 239 Np tracer.

[0039] The radioactive solution of americium and neptunium is rich in sodium nitrite. 243 Am and its decay daughters 239 A solution composed of Np.

[0040] The acid in step 1 is nitric acid, hydrochloric acid, hydrofluoric acid or a combination of the above acids, and the concentration of the acid is 0.01 to 8.0 mol / L.

[0041] The radioactive solution containing americium and neptunium is 4-8 mol / L HNO3; the aqueous washing solution is 4-8 mol / L HNO3 solution; the first-stage eluent is 0.01-0.5 mol / L HNO3 solution; the second-stage eluent is 0.05-0.2 mol / L HCl solution; the third-stage eluent is 0.05-0.2 mol / L HCl solution containing 0.05-0.5 mol / L HF.

[0042] The TODGA column and LN or P 204 or P 507 The chromatographic column can be automatically regenerated and used in the next preparation process.

[0043] The above-mentioned first separation preparation 239 After Np, the recovered radioactive solution of americium is completely consistent with the acid composition and concentration of the radioactive solution of americium and neptunium required before preparation, and directly meets the conditions for the next preparation.

[0044] The above-mentioned preparation cycle is repeated 10 times, after which the chromatography adsorption column needs to be replaced.

[0045] The americium separated and recovered is stored in a liquid storage tank rather than on a chromatography column.

[0046] The americium-neptunium radioactive solution storage tank is provided with a shielding body outside.

[0047] The above separation and preparation process is carried out at room temperature.

[0048] The beneficial effects of the present invention are:

[0049] A double column circulation preparation 239 The device of Np tracer effectively utilizes the characteristics of two chromatographic columns to adsorb americium and neptunium, and cleverly matches the connection between the output and input solutions of the two columns, so that the TODGA chromatographic adsorption column can prepare high-purity 239 Np tracer, LN or P 204 or P 507 Chromatographic column conversion 243The Am solution system is the starting liquid medium, laying the foundation for the automated control and cyclic preparation of the process.

[0050] A double column circulation preparation 239 Device for recovering Np tracer 243 The Am solution is automatically stored in a radiation-shielded storage tank instead of being retained on the chromatographic separation column, which avoids the radiation degradation of the organic adsorption material, provides effective protection for the multiple recycling use of the chromatographic separation column, and ensures the radiation safety of personnel.

[0051] A double column circulation preparation 239 The method of Np tracer has clear functions of each separation unit, simple process, easy control and adjustment, integrated design of separation, purification, preparation, medium conversion, regeneration and other processes. The whole process can be completed within 1.5 hours and can achieve ten times 239 Cyclic preparation of Np tracers.

[0052] A double column circulation preparation 239 Compared with the existing methods, the Np tracer method realizes the program-controlled automatic separation of americium and neptunium; 239 Np and 243 The recovery rate of Am is better than 95% and 99%, 239 The radioactivity purity of Np is 99.9993%, and the decontamination factor of americium to neptunium is 10 5 . BRIEF DESCRIPTION OF THE DRAWINGS

[0053] Figure 1 The double column circulation preparation of the present invention 239 Schematic diagram of the Np tracer device;

[0054] Figure 2 For Example 1 of the present invention, 243 Am and 239 γ-radioactivity spectrum of Np mother and daughter original solution;

[0055] Figure 3 Separated from Example 1 of the present invention 239 γ-radioactivity spectrum of Np tracer;

[0056] Figure 4 After separation using Example 1 of the present invention 243 Gamma-radiation energy spectrum of Am.

[0057] Reference numerals: 1-feed liquid reservoir, 2-washing liquid reservoir, 3-first stage eluent reservoir, 4-second stage eluent reservoir, 5-third stage eluent reservoir, 6-product collector, 7-waste liquid collector, 8-TODGA chromatography adsorption column, 9-LN or P 204 or P 507Chromatographic adsorption column, 10-valve, 11-delivery pump, 12-temperature controller, 13-radiation shielding body. DETAILED DESCRIPTION

[0058] The present invention is further described in detail below with reference to the accompanying drawings and specific embodiments.

[0059] like Figure 1 As shown, the double column circulation preparation of the present invention 239 The device of Np tracer includes a temperature controller 12, a radiation shield 13, a liquid storage tank unit, a chromatographic separation unit, a waste liquid collector 7, and a product collector 6. The above units and devices are connected by pipelines. Preferably, the pipeline adopts a silicone tube; and corresponding valves 10 and a delivery pump 11 are configured in the pipeline. In this way, the electromagnetic valve and the peristaltic pump can be controlled by a microcomputer to realize automatic control of the separation process, reduce the impact of radioactive nuclide radiation on the human body during separation, and reduce the labor intensity of personnel. The peristaltic pump uses a hose extrusion method to deliver the separation liquid, and the flow rate and flow velocity of the liquid are controlled by the rotation speed of the peristaltic pump.

[0060] The above-mentioned liquid storage tank unit includes a feed liquid storage tank 1, a washing liquid storage tank 2, a first-stage eluent storage tank 3, a second-stage eluent storage tank 4, and a third-stage eluent storage tank 5. Each storage tank is connected to a corresponding chromatographic adsorption column through a valve and a pump, and realizes different functions;

[0061] The above-mentioned chromatographic separation unit includes a TODGA chromatographic adsorption column 8, LN or P 204 or P 507 Chromatographic adsorption column 9.

[0062] The connection relationship between the above-mentioned liquid storage tanks and the chromatographic adsorption column is as follows: the feed liquid storage tank 1 is placed at the lower end, and its internal bottom end is connected to the inlet of the delivery pump through a pipeline and a valve; the washing liquid storage tank 2, the first-stage eluent storage tank 3, the second-stage eluent storage tank 4 and the third-stage eluent storage tank 5 are placed in parallel at the upper end, and their outlets are connected to the inlet of the delivery pump 11 through a valve 10; the outlet of the delivery pump 11 is connected to the TODGA chromatographic adsorption column 8 and the LN or P through the valve 10, respectively. 204 or P 507 The discharge port of the TODGA chromatographic adsorption column 8 is connected to the waste liquid collector 7, LN or P through valve 10 respectively. 204 or P 507 The inlet of the chromatographic adsorption column 9 is connected to the product collector 6; LN or P 204 or P 507 The discharge port of the chromatography adsorption column 9 is connected to the waste liquid collector 7 and the feed liquid storage tank 1 through a valve 10 respectively.

[0063] The separation step of the present invention is:

[0064] Step 1: Preparation before separation

[0065] 100 mg of sodium nitrite is added to the radioactive solution containing americium and neptunium, and the solution is kept at a constant temperature of 70 to 100 degrees for 15 minutes and then cooled to form a feed solution before separation; the acid is dissolved in water to form an aqueous washing solution and an aqueous eluent; the acid used is nitric acid and hydrochloric acid, hydrofluoric acid or a combination of the above acids, and the concentration of the acid is 0.01 to 8.0 mol / L; TODGA, LN or P 204 or P 507 The resins are loaded into chromatography columns respectively.

[0066] The TODGA column is used to separate Np from Am and constant Na; LN or P 204 or P 507 The chromatographic column is used to convert the acid system of eluting and recovering Am into the acid composition and concentration required before the radioactive solution of americium and neptunium is separated on the column, so that it can be directly used for the next 239 Np tracer preparation.

[0067] Step 2: using a peristaltic pump to deliver and a solenoid valve to select, the radioactive solution containing americium and neptunium passes through the TODGA chromatography adsorption column 8 to adsorb americium and neptunium, and the effluent is collected as waste liquid;

[0068] Step 3: Use a peristaltic pump to deliver and an electromagnetic valve to select, so that the washing liquid passes through the TODGA chromatography adsorption column 8 for washing, adsorption and separation, and the effluent is collected as waste liquid;

[0069] Step 4: Use a peristaltic pump to deliver and a solenoid valve to select so that the first-stage eluent passes through the TODGA chromatography adsorption column 8 to desorb neptunium; the effluent, i.e., the radioactive solution of neptunium, is collected in the product collector 6;

[0070] Step 5: Use the peristaltic pump to deliver and the solenoid valve to select, so that the second-stage eluent passes through the TODGA chromatography adsorption column 8 and LN or P in turn. 204 or P 507 The chromatographic adsorption column 9 performs desorption and re-adsorption of americium, and the effluent is collected as waste liquid;

[0071] Step 6: Use the peristaltic pump to deliver and the solenoid valve to select, so that the first-stage eluent passes through LN or P 204 or P 507 The chromatographic adsorption column 9 is washed, and the effluent is collected as waste liquid;

[0072] Step 7: Use the peristaltic pump to deliver and the solenoid valve to select, so that the washing liquid passes through LN or P 204 or P 507The chromatographic adsorption column 9 desorbs americium, and the effluent, i.e., the radioactive solution of americium, is collected in the storage tank 1 for the radioactive solution of americium and neptunium;

[0073] Step 8: Use a peristaltic pump to deliver and a solenoid valve to select, so that the third-stage eluent passes through the TODGA chromatography adsorption column 8, and the effluent is collected as waste liquid;

[0074] Step 9: Use the peristaltic pump to deliver and the solenoid valve to select the second-stage eluent through LN or P 204 or P 507 The pipeline between the chromatography adsorption column 9 and the TODGA chromatography adsorption column 8, the outflow liquid is collected as waste liquid;

[0075] Step 10: Use the peristaltic pump to deliver and the solenoid valve to select the second-stage eluent through LN or P 204 or P 507 Chromatographic adsorption column 9, the effluent is collected as waste liquid;

[0076] Step 11: Use a peristaltic pump to deliver and a solenoid valve to select, so that the washing liquid passes through the TODGA chromatography adsorption column 8, and the effluent is collected as waste liquid;

[0077] Step 12: After the americium solution in the americium-neptunium radioactive solution storage tank is left for 7 to 8 days, sufficient new 239 Np, repeat the first step to the eleventh step, enter the next preparation process, and cycle through the preparation in this way 239 Np tracer.

[0078] In the above method, the radioactive solution of americium and neptunium is rich in sodium nitrite. 243 Am and its decay daughters 239 A solution composed of Np.

[0079] The specific embodiments are as follows:

[0080] Example 1

[0081] Add 100 mg of sodium nitrite to 15 mL of 5 mol / L HNO3 americium-neptunium radioactive solution in the liquid storage tank 1, and maintain the temperature at 80 degrees for 15 minutes and cool to form a feed solution before separation. Its γ radioactivity spectrum is as follows: Figure 2 shown.

[0082] The flow rate of the americium-neptunium feed solution is controlled at 1.5 mL / min, and the americium-neptunium solution is separated by a TODGA chromatographic adsorption column 8. The TODGA chromatographic adsorption column is A TODGA chromatography column is used to separate americium and neptunium from the major element Na, and the effluent is collected in a waste liquid collector 7.

[0083] Use 15 mL of 5 mol / L HNO3 solution in the washing liquid reservoir 2 to wash through the TODGA chromatography adsorption column 8 at a flow rate of 2 mL / min, and collect the effluent in the waste liquid collector 7.

[0084] Use 12mL 0.1mol / L HNO3 solution in the first-stage eluent reservoir 3, control the flow rate to 1.5mL / min, and pass through the TODGA chromatography adsorption column 8 to desorb neptunium; the effluent, i.e. the radioactive solution of neptunium, is collected in the product collector 6, and its γ radioactivity spectrum is as follows Figure 3 shown.

[0085] Use 15 mL of 0.1 mol / L HCl solution in the second-stage eluent reservoir 4, control the flow rate to 1.5 mL / min, and sequentially pass through the TODGA chromatography adsorption column 8 and the LN chromatography adsorption column to desorb and re-adsorb americium, wherein the LN chromatography adsorption column is The LN chromatography column is used to achieve the adsorption of Am, and the effluent is collected as waste liquid.

[0086] Use 5 mL of 0.1 mol / L HNO3 solution in the first-stage eluent reservoir 3, control the flow rate to 1.5 mL / min, wash through the LN chromatography adsorption column, and collect the effluent as waste liquid.

[0087] Use 15mL 5mol / L HNO3 solution in the washing liquid reservoir 2, control the flow rate to 1.5mL / min, and desorb americium through the LN chromatography adsorption column. The effluent, i.e. the radioactive solution of americium, is collected in the americium-neptunium radioactive solution reservoir 1. Its γ radioactivity spectrum is as follows: Figure 4 shown.

[0088] Use 10 mL of 0.1 mol / L HCl-0.3 mol / L HF solution in the third-stage eluent reservoir 5, control the flow rate to 1.5 mL / min, pass through the TODGA chromatography adsorption column 8, and collect the effluent as waste liquid.

[0089] Use 5 mL of 0.1 mol / L HCl solution in the second-stage eluent reservoir 4, control the flow rate to 2 mL / min, pass through the pipeline between the LN chromatography adsorption column and the TODGA chromatography adsorption column 8, and collect the effluent as waste liquid.

[0090] Use 15 mL of 0.1 mol / L HCl solution in the second-stage eluent reservoir 4, control the flow rate to 2 mL / min, pass through the LN chromatography adsorption column, and collect the effluent as waste liquid.

[0091] Use 15 mL of 5 mol / L HNO3 solution in the washing liquid reservoir 2, control the flow rate to 2 mL / min, pass through the TODGA chromatography adsorption column 8, and collect the effluent as waste liquid.

[0092] 239 Np and 243 The recovery rates of Am were 95.6% and 99.7% respectively, and the separation process took 85 minutes. 239 Np decays completely, identification 239 The Np radioactivity purity is 99.9993%.

[0093] Example 2

[0094] The americium-neptunium radioactive solution storage tank in Example 1 243 After the Am solution was left for 7 days, the separation process of Example 1 was repeated to obtain 239 Np tracer and for next cycle use 243 Am solution. Measured 239 The Np recovery rate was 95.8%, 239 The radioactivity purity of Np is 99.9992%. 243 The recovery rate of Am was 99.5%.

[0095] Example 3

[0096] The LN chromatography column in Example 1 was replaced by P 204 Chromatographic adsorption column, repeat the separation process of Example 1, and obtain 239 Np tracer and for next cycle use 243 Am solution. Measured 239 The Np tracer recovery rate was 95.1%, 239 The radioactivity purity of Np is 99.9992%. 243 The recovery rate of Am was 99.4%. 239 The decontamination factor of americium to neptunium determined by Np decontamination experiment is 1.3×10 5 .

Claims

1. A double column circulation preparation 239 The device of Np tracer is characterized in that It includes a temperature controller (12), a radiation shield (13), a liquid storage tank unit, a chromatography separation unit, a waste liquid collector (7), a product collector (6), a valve (10) and a delivery pump (11) assembly; The liquid in the liquid storage tank unit enters the chromatographic separation unit through a delivery pump (11), and the liquid flowing out of the chromatographic separation unit enters a waste liquid collector (7) or a product collector (6) or a feed liquid storage tank (1); the components through which the liquid in the liquid storage tank unit flows are connected by pipelines, and valves (10) are provided on the pipelines through which the liquid flows through each component; The liquid storage tank unit comprises a feed liquid storage tank (1), a washing liquid storage tank (2), a first-stage eluent storage tank (3), a second-stage eluent storage tank (4), and a third-stage eluent storage tank (5), and each storage tank is connected to the chromatographic separation unit via a valve (10) and a delivery pump (11); The liquid storage tank (1) is located inside a temperature controller (12), and a radiation shielding body (13) is arranged outside the temperature controller (12); The chromatographic separation unit comprises a TODGA chromatographic adsorption column (8), LN or P 204 or P 507 Chromatographic adsorption column (9); TODGA chromatography column (8) is used to separate Np from Am and constant Na, LN or P 204 or P 507 The chromatographic adsorption column (9) is used for eluting and recovering americium; The connection relationship between the liquid storage tank unit and the chromatographic separation unit is as follows: the feed liquid storage tank (1) is placed at the lower end, and its internal bottom end is connected to the inlet of the delivery pump through a pipeline and a valve; the washing liquid storage tank (2), the first-stage eluent storage tank (3), the second-stage eluent storage tank (4) and the third-stage eluent storage tank (5) are placed in parallel at the upper end, and their outlets are connected to the inlet of the delivery pump (11) through a valve (10); the outlet of the delivery pump (11) is respectively connected to the TODGA chromatographic adsorption column (8) and the LN or P through the valve (10). 204 or P 507 The discharge port of the TODGA chromatographic adsorption column (8) is connected to the waste liquid collector (7), LN or P through a valve (10). 204 or P 507 The inlet of the chromatographic adsorption column (9) is connected to the product collector (6); LN or P 204 or P 507 The discharge port of the chromatographic adsorption column (9) is respectively connected to the waste liquid collector (7) and the feed liquid storage tank (1) through a valve (10).

2. Double column circulation preparation according to claim 1 239 The device of Np tracer is characterized in that The pipeline is a silicone tube.

3. The double column circulation preparation according to claim 1 239 The device of Np tracer is characterized in that It also includes a microcomputer, which is used to control the valve (10) and the delivery pump (11); The valve (10) is a solenoid valve, and the delivery pump (11) is a peristaltic pump; the rotation speed of the peristaltic pump controls the flow rate and flow velocity of the liquid.

4. A double column circulation preparation 239 The method of Np tracer, characterized in that The following steps are involved: Step 1, preparation before separation: Placing the radioactive solution of americium and neptunium to be separated into a feed liquid storage tank (1), adding sodium nitrite, controlling the temperature of the feed liquid storage tank (1) to be 70° to 100° by a temperature controller (12), keeping the temperature for a certain period of time, and cooling to room temperature to obtain a feed liquid containing americium and neptunium; Dissolve nitric acid and hydrochloric acid, hydrofluoric acid or a combination of the above acids at a concentration of 0.01 mol / L to 8.0 mol / L in water respectively. A washing liquid and an eluent are formed, and both the washing liquid and the eluent are aqueous; TODGA, LN, P 204 , P 507 The resins are respectively loaded into chromatographic columns to obtain corresponding chromatographic adsorption columns; Step 2, adsorption of americium and neptunium: The feed liquid in the feed liquid storage tank (1) passes through a TODGA chromatographic adsorption column (8), so that americium and neptunium are adsorbed in the TODGA chromatographic adsorption column (8), and the effluent of the TODGA chromatographic adsorption column (8) is collected in a waste liquid collector (7); Step 3, washing: The washing liquid in the washing liquid storage tank (2) passes through a TODGA chromatographic adsorption column (8) for washing, and the effluent of the TODGA chromatographic adsorption column (8) is collected in a waste liquid collector (7); Step 4: Rinse: First, the first-stage eluent in the first-stage eluent storage tank (3) is passed through a TODGA chromatography adsorption column (8) for elution, and the effluent of the TODGA chromatography adsorption column (8) is collected in a product collector (6) to obtain a neptunium radioactive solution; Secondly, the second-stage eluent in the second-stage eluent storage tank (4) passes through the TODGA chromatography adsorption column (8) and LN or P in sequence. 204 or P 507 Chromatographic adsorption column (9) for desorption and re-adsorption of americium, LN or P 204 or P 507 The effluent from the chromatography adsorption column (9) is collected in a waste liquid collector (7); Again, the washing liquid in the washing liquid storage tank (2) is passed through LN or P 204 or P 507 Chromatographic adsorption column (9) is used to desorb americium and to remove LN or P 204 or P 507 The effluent from the chromatographic adsorption column (9) is collected in the feed liquid storage tank (1).

5. The double column circulation preparation according to claim 4 239 The method of Np tracer, characterized in that It also includes step five, regeneration, the specific process is: First, the third-stage eluent in the third-stage eluent storage tank (5) passes through a TODGA chromatography adsorption column (8), and the effluent of the TODGA chromatography adsorption column (8) is collected in a waste liquid collector (7); Secondly, the second-stage eluent in the second-stage eluent storage tank (4) is passed through LN or P 204 or P 507 The pipeline between the chromatography adsorption column (9) and the TODGA chromatography adsorption column (8) flows into the waste liquid collector (7); Again, the second-stage eluent in the second-stage eluent storage tank (4) is passed through LN or P 204 or P 507 Chromatographic adsorption column (9), LN or P 204 or P 507 The effluent from the chromatographic adsorption column (9) is collected in the waste liquid collector (7); finally, the washing liquid in the washing liquid storage tank (2) passes through the TODGA chromatographic adsorption column (8), and the effluent from the TODGA chromatographic adsorption column (8) is collected in the waste liquid collector (7).

6. The double column circulation preparation according to claim 4 239 The method of Np tracer, characterized in that The amount of HNO3 contained in the americium-neptunium liquid is 4 mol / L to 8 mol / L.

7. The double column circulation preparation according to claim 4 239 The method of Np tracer, characterized in that The step 1, preparation before separation, further comprises: A 4mol / L to 8mol / L HNO3 solution is used as a washing liquid, and the washing liquid is placed in a washing liquid storage tank (2); a 0.01mol / L to 0.5mol / L HNO3 solution is used as a first-stage eluent, and the first-stage eluent is placed in a first-stage eluent storage tank (3); a 0.05mol / L to 0.2mol / L HCl solution is used as a second-stage eluent, and the second-stage eluent is placed in a second-stage eluent storage tank (4); a 0.05mol / L to 0.2mol / L HCl solution containing 0.05mol / L to 0.5mol / L HF is used as a third-stage eluent, and the third-stage eluent is placed in a third-stage eluent storage tank (5).

8. The double column circulation preparation according to claim 4 239 The method of Np tracer, characterized in that In the preparation before separation of step 1, the radioactive americium-neptunium solution to be separated is 15 mL of a radioactive americium-neptunium solution containing 5 mol / L HNO3, 100 mg of sodium nitrite is added, and the temperature of the feed liquid storage tank (1) is controlled by a temperature controller (12) to be 80°, and the temperature is kept for 15 minutes; In the adsorption of americium and neptunium in step 2, the flow rate of the feed liquid is 1.5 mL / min, and the feed liquid passes through the TODGA chromatographic adsorption column (8). The TODGA chromatographic adsorption column (8) is In the step 3, the washing liquid is 15 mL of a 5 mol / L HNO3 solution, the flow rate is 2 mL / min, and the washing liquid passes through a TODGA chromatography adsorption column (8); In the first process of step 4, the first-stage eluent is 12 mL of 0.1 mol / L HNO3 solution at a flow rate of 1.5 mL / min, which passes through a TODGA chromatographic adsorption column (8); in the second process of step 4, the second-stage eluent is 15 mL of 0.1 mol / L HCl solution at a flow rate of 1.5 mL / min, which passes through a TODGA chromatographic adsorption column (8) and an LN chromatographic adsorption column to desorb and re-adsorb americium. The LN chromatographic adsorption column is In the second process of step 4, the first-stage eluent is 5 mL of 0.1 mol / L HNO3 solution at a flow rate of 1.5 mL / min, which passes through a LN chromatographic adsorption column; in the final process of step 4, the washing liquid is 15 mL of 5 mol / L HNO3 solution at a flow rate of 1.5 mL / min, which desorbs americium through a LN chromatographic adsorption column.

9. The double column circulation preparation according to claim 5 239 The method of Np tracer, characterized in that In the first process of step 5, the third-stage eluent is 10 mL of 0.1 mol / L HCl-0.3 mol / L HF solution, and the flow rate is 1.5 mL / min, passing through the TODGA chromatography adsorption column (8); In the second process of step 5, the second-stage eluent is 5 mL of 0.1 mol / L HCl solution at a flow rate of 2 mL / min; it passes through the pipeline between the LN chromatography adsorption column and the TODGA chromatography adsorption column (8); In the process of step 5, the second eluent is 15 mL of 0.1 mol / L HCl solution, the flow rate is 2 mL / min, and the second eluent passes through the LN chromatography adsorption column; In the final process of step 5, the washing liquid is 15 mL of 5 mol / L HNO3 solution, and the flow rate is 2 mL / min, and the washing liquid passes through the TODGA chromatography adsorption column (8).

10. The double column circulation preparation according to claim 4 239 The method of Np tracer, characterized in that The americium-neptunium radioactive solution is rich in sodium nitrite. 243 Am and its decay daughters 239 A solution composed of Np.

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