An apparatus and method for separating trivalent actinide and fission product nuclides

Abstract

The present application relates to a kind of trivalent actinide and rare earth fission fragment nuclide separation device and separation method, belong to actinide and fission product separation technical field, solve the technical problem that separation exists decontamination low, recovery rate is low, its separation device includes liquid storage tank unit, chromatography separation unit, waste liquid collector, product collection unit, delivery pump.Liquid of liquid storage tank unit enters chromatography separation unit by delivery pump, the liquid that chromatography separation unit flows enters waste liquid collector or product collection unit.Liquid storage tank unit, chromatography separation unit, product collection unit, waste liquid collector are connected by pipeline, on pipeline, set valve.Its separation method includes preparation before separation, the steps of adsorption, washing, leaching of trivalent actinide and rare earth fission fragment nuclide.The present application is used for the separation of trivalent actinide and rare earth fission fragment nuclide.

Description

Technical Field

[0001] The invention belongs to the technical field of separation of actinides and fission products, and in particular relates to a device and a method for separating trivalent actinides and rare earth fragment nuclides. Background Art

[0002] Radiochemical analysis of activation and fission products in spent fuel solutions can determine reactor burnup and neutron flux. The plutonium isotope Pu-241 has a half-life of 14.29 years and undergoes radioactive decay to produce the daughter Am-241 with a half-life of 432.2 years. Neutrons activate Am-241, which then decays into Cm-242 (half-life of 163 days). Analysis and measurement of americium-curium isotopes can provide information on neutron flux. Fissile nuclides such as uranium and plutonium undergo fission reactions under the action of neutrons, producing hundreds of radioactive fission products. Among them, rare earth fragment nuclides such as Ce-141 (half-life 32.4 days) and Ce-144 (half-life 284 days), Nd-147 (half-life 11.1 days), Sm-153 (half-life 46.8 hours), Eu-155 (half-life 4.96 years) and Eu-156 (15.2 days), terbium fission product Tb-161 (half-life 6.91 days), etc., have half-lives ranging from tens of hours to several years, making them suitable for long-term monitoring and analysis. Moreover, their fission yields cover a wide range, from extremely low Tb-161 (9.2×10 -5 %) to Ce-141 with a high yield (5.98%), becoming the fission product of focus in reactor burnup monitoring analysis and fission yield determination.

[0003] Americium and curium isotopes are typically measured using semiconductor alpha spectrometry and mass spectrometry. However, due to the relatively low energy resolution of semiconductor alpha spectrometers, the Cm-242 peak at 6.113 MeV causes strong peak tailing interference on the Am-241 peak at 5.485 MeV. Furthermore, mass spectrometry results in interference from Cm-242 isotopes in Am-242m. Accurate measurement and analysis of americium and curium isotopes requires resolving the mutual separation of americium and curium isotopes. Gamma-ray fission products of rare earth fragments, such as Ce-141, Ce-144, Nd-147, Sm-153, Eu-155, Eu-156, and Tb-161, each produce multiple gamma rays. Consequently, activity measurements using high-purity germanium trap-type gamma spectrometers can be subject to varying degrees of interference from repeated peaks and cross-peaks. Furthermore, the uranium-plutonium fission process produces a large number of other fission products that are rich in gamma rays, such as Mo-99, Tc-99m, Te-132, Ru-103, I-131, I-132, Ba-140, La-140, Zr-95, and Nb-95. These products cause significant interference with the Compton plateau and spectral peaks, affecting the accurate measurement of low-activity nuclides. Therefore, it is necessary to separate and prepare radiochemically pure rare earth fragments for measurement.

[0004] Perna et al. (Studies on simultaneous separation and determination of lanthanides and actinides by ion chromatography inductively coupled plasma mass spectrometry combined with isotope dilution mass spectrometry, J. Anal. At. Spectrom., 2002, 17:1166-1171) reported the simultaneous separation and purification of actinides uranium, plutonium, and americium from spent fuel samples using mixed-bed ion chromatography (Dionex CS5A), and the determination of their contents by isotope dilution mass spectrometry. However, this separation method was only sufficient for the measurement of stable lanthanide fission products (Ce-140, Nd-143, Nd-146, Sm-150, Eu-153, etc.), failing to resolve the separation of gamma-radioactive lanthanide fission products from other interfering nuclides, nor did it address the separation of americium from curium.

[0005] Modolo et al. (Demonstration of the LUCA process for the separation of americium(III) from curium(III), californium(III), and lanthanides(III) in acidic solution using a synergistic mixture of bis(chrophenyl)dithiophosphinic acid and tris(2-ethylhexyl)phosphate. Radiochim. Acta, 2010, 98:193-201.) reported the selective separation of trivalent americium, trivalent curium, and the rare earth element europium from an acidic solution using a liquid-liquid extraction process comprising seven extraction stages, nine washing stages, and eight stripping stages using multiple centrifugal extractors. However, the separation of other rare earth fragments was not mentioned. Furthermore, the method required expensive experimental equipment and a complex process, making it unsuitable for analysis of laboratory samples.

[0006] Arrigo et al., "Separation of lanthanide isotopes from mixed fission product samples." Separations., 2021, 8:104-114, reported the use of UTEVA-TRU-LN resin chromatography to separate and extract gamma-radioactive lanthanide fission products (Ce-144, Sm-153, Eu-156, Tb-161, etc.) from mixed fission products of uranium irradiation for their cumulative fission yield measurement. However, the recovery rate of the low-yield nuclide Eu-156 was not high (56%), and the decontamination factor for the high-yield nuclide Nd-147 was less than 3.8×10 3 The incomplete separation and decontamination of lanthanide fission products from each other and from other fission products results in a large uncertainty in yield determination (10.9% to 22.7%). This method does not meet the technical requirements for high-precision analysis of americium curium and rare earth fragment nuclides. Summary of the Invention

[0007] In order to overcome the shortcomings of low decontamination and low recovery rate in the separation of trivalent actinides and rare earth fragment nuclides, the present invention provides a separation device and a separation method for trivalent actinides and rare earth fragment nuclides.

[0008] The technical solution adopted by the present invention to solve the technical problem is:

[0009] A device for separating trivalent actinide elements and rare earth fragment nuclides comprises a liquid storage tank unit, a chromatography separation unit, a waste liquid collector, a product collection unit, and a delivery pump.

[0010] The liquid of the liquid storage tank unit is pumped into the chromatographic separation unit, and the liquid flowing out of the chromatographic separation unit is pumped into the waste liquid collector or the product collection unit;

[0011] The liquid storage tank unit, the chromatographic separation unit, the product collection unit and the waste liquid collector are connected by pipelines, and valves are arranged on the pipelines through which the liquid flows;

[0012] The liquid storage tank unit is located at the uppermost end, and the waste liquid collector and the product collection unit are located at the lowermost end;

[0013] The liquid storage tank unit includes a trivalent actinide and rare earth fission fragment nuclide radioactive solution storage tank, a washing liquid storage tank, a first-stage column eluent storage tank, a second-stage column first-stage eluent storage tank, a second-stage column second-stage eluent storage tank, a second-stage column third-stage eluent storage tank, a second-stage column fourth-stage eluent storage tank, a second-stage column fifth-stage eluent storage tank, a second-stage column sixth-stage eluent storage tank, a third-stage column first-stage eluent storage tank, a third-stage column second-stage eluent storage tank, a third-stage column third-stage eluent storage tank, a fourth-stage column first-stage eluent storage tank, a fourth-stage column second-stage eluent storage tank, and a fourth-stage column third-stage eluent storage tank, which are located on the same horizontal plane.

[0014] The chromatographic separation unit includes, from top to bottom, an RE or TRU chromatographic adsorption column, a P 204 or HDEHP chromatographic adsorption column, a DN chromatographic adsorption column, and a BCPDTPA chromatographic adsorption column. 204 The lower end of the P 204 or HDEHP chromatographic adsorption column is connected to the third-stage column first-stage eluent storage tank through a pipeline.

[0015] The product collection unit includes, on the same horizontal plane, a cymatium product collector, an americium product collector, a cerium product collector, a terbium product collector, a samarium product collector, an europium product collector, and a neodymium product collector. The waste liquid collector is located on the same horizontal plane as the chromatographic separation unit.

[0016] In the above separation device, the valves are solenoid valves, the delivery pumps are peristaltic pumps, and the pipelines are silica gel tubes.

[0017] The above separation device further includes a microcomputer, which is used to control the solenoid valves and the peristaltic pumps.

[0018] In the above separation device, the connection relationship between the liquid storage tank unit, the chromatographic separation unit, the waste liquid collector, and the product collection unit is as follows:

[0019] The outlets of the radioactive solution reservoir containing trivalent actinides and rare earth fragment nuclides, the washing liquid reservoir, the first column eluent reservoir, the second column first eluent reservoir, the second column second eluent reservoir, the second column third eluent reservoir, the second column fourth eluent reservoir, the second column fifth eluent reservoir, the second column sixth eluent reservoir, the third column first eluent reservoir, the third column second eluent reservoir, the third column third eluent reservoir, the fourth column first eluent reservoir, the fourth column second eluent reservoir, and the fourth column third eluent reservoir are connected to the corresponding inlets of the delivery pump through valves; the outlets of the delivery pump are respectively connected to the RE or TRU chromatographic adsorption column, the P 204 Or HDEHP chromatography adsorption column, BCPDTPA chromatography adsorption column, DN chromatography adsorption column inlet connection; RE or TRU chromatography adsorption column outlet through the valve and P 204 Or connect the HDEHP chromatography adsorption column feed port and waste liquid collector; 204 Or the discharge port of the HDEHP chromatography adsorption column is connected to the inner bottom end of the third-stage eluent storage tank of the third-stage column, the cerium product collector, the terbium product collector, the DN chromatography adsorption column feed port and the waste liquid collector through valves; the discharge port of the BCPDTPA chromatography adsorption column is connected to the curium product collector, the americium product collector and the waste liquid collector through valves; the discharge port of the DN chromatography adsorption column is connected to the samarium product collector, the europium product collector, the neodymium product collector and the waste liquid collector through valves.

[0020] A method for separating trivalent actinide elements and rare earth fragment nuclides comprises the following steps:

[0021] Step 1, preparation before separation

[0022] The radioactive sample containing trivalent actinides and rare earth fragments to be separated is dissolved in nitric acid, sodium nitrite is added, and the mixture is heated at 90 to 100° C. and then cooled to obtain an aqueous radioactive sample containing trivalent actinides and rare earth fragments;

[0023] The washing and rinsing acids are dissolved in water to obtain an aqueous washing solution and an aqueous rinsing solution respectively; the washing and rinsing acids are selected from nitric acid, hydrochloric acid, or a mixture of diethylenetriaminepentaacetic acid and lactic acid;

[0024] RE or TRU resin, P 204 Or HDEHP resin, BCPDTPA resin, DN resin are respectively loaded into chromatography adsorption column to obtain RE or TRU chromatography adsorption column, P 204 Or HDEHP chromatography adsorption column, BCPDTPA chromatography adsorption column, DN chromatography adsorption column;

[0025] Step 2, adsorption of trivalent actinides and rare earth fragments

[0026] The aqueous radioactive sample containing trivalent actinides and rare earth fragments prepared in step 1 is placed in a reservoir of radioactive solution containing trivalent actinides and rare earth fragments, and the radioactive sample containing actinides and lanthanide fission products is separated and adsorbed using a RE or TRU chromatographic adsorption column. The trivalent actinides and rare earth fragments are adsorbed in the RE or TRU chromatographic adsorption column, and the effluent is collected into a waste liquid collector.

[0027] Step 3, washing

[0028] Use aqueous washing solution to wash the RE or TRU chromatography adsorption column and collect the effluent into the waste liquid collector;

[0029] Step 4, rinse

[0030] Use aqueous eluent to wash RE or TRU chromatography column, P 204 Or a HDEHP chromatography adsorption column, a DN chromatography adsorption column, and a BCPDTPA chromatography adsorption column are used for elution to obtain a γ-radioactive solution of cerium, a γ-radioactive solution of terbium, a γ-radioactive solution of americium, a γ-radioactive solution of curium, a γ-radioactive solution of neodymium, a γ-radioactive solution of samarium, and a γ-radioactive solution of europium.

[0031] In the above separation method, in the preparation before separation in step 1, the concentration of nitric acid used to dissolve the radioactive sample of trivalent actinides and rare earth fragments to be separated is 1 mol / L to 4 mol / L, and the concentration of the acid used for washing and eluting is 0.01 to 10 mol / L.

[0032] In the above separation method, in the preparation before separation in step 1, the aqueous washing liquid is a 1 mol / L to 4 mol / L HNO3 solution, and the aqueous washing liquid is placed in a washing liquid storage tank.

[0033] In the above-mentioned separation method, in the preparation before separation in step 1, the aqueous eluent includes the eluent of the first column, the first eluent of the second column, the second eluent of the second column, the third eluent of the second column, the fourth eluent of the second column, the fifth eluent of the second column, the sixth eluent of the second column, the first eluent of the third column, the second eluent of the third column, the third eluent of the third column, the first eluent of the fourth column, the second eluent of the fourth column, and the third eluent of the fourth column, and the above-mentioned eluents are placed in corresponding liquid storage tanks.

[0034] The first column eluent was 0.05 mol / L HNO3 solution at a flow rate of 1.0 mL / min;

[0035] The first-stage eluent of the second-stage column is 0.1 mol / L HNO3 solution with a flow rate of 1.0 mL / min;

[0036] The second-stage eluent of the second-stage column was 0.05 mol / L DTPA-1 mol / L lactic acid solution, pH 3.0, with a flow rate of 1.0 mL / min;

[0037] The third eluent of the second column was 0.2 mol / L HNO3-0.07 mol / L NaBrO3 solution at a flow rate of 1.0 mL / min;

[0038] The fourth eluent of the second column was 1 mol / L HNO3-0.07 mol / L NaBrO3 solution with a flow rate of 1.0 mL / min;

[0039] The fifth stage eluent of the second column was 1 mol / L HNO3 solution with a flow rate of 1.0 mL / min;

[0040] The sixth stage eluent of the second stage column is 3 mol / L HNO3 solution with a flow rate of 0.5 mL / min;

[0041] The first-stage eluent of the third-stage column was 0.05 mol / L TPA-1 mol / L lactic acid solution at a flow rate of 1.0 mL / min;

[0042] The second-stage eluent of the third-stage column is 0.1 mol / L HNO3 solution with a flow rate of 1.0 mL / min;

[0043] The third-stage eluent of the third-stage column is 1 mol / L HNO3 solution with a flow rate of 1.0 mL / min;

[0044] The first-stage eluent of the fourth-stage column was 2.75 mol / L HCl solution with a flow rate of 1.0 mL / min;

[0045] The second-stage eluent of the fourth-stage column was 1.5 mol / L HCl solution with a flow rate of 0.5 mL / min;

[0046] The third-stage eluent of the fourth-stage column is 0.1 mol / L HCl solution, and the flow rate is 0.5 mL / min.

[0047] In the above separation method, the step 4 of eluting further comprises:

[0048] The first column eluent passes through the RE or TRU chromatography adsorption column and P 204 Or HDEHP chromatography adsorption column, to desorb and re-adsorb trivalent actinides and rare earth fragment nuclides, and collect the effluent into the waste liquid collector;

[0049] The first stage eluent of the second stage column passes through P 204 Or HDEHP chromatography adsorption column, wash, and collect the effluent into the waste liquid collector;

[0050] The second stage eluent of the second stage column passes through P 204 Or HDEHP chromatography adsorption column, desorption of trivalent actinide, the effluent is collected into the first stage eluent reservoir 0 of the third stage column;

[0051] The second column and the third stage eluent pass through P 204 Or HDEHP chromatography adsorption column, wash, and collect the effluent into the waste liquid collector;

[0052] The second column and the fourth stage eluent pass through P 204 Or HDEHP chromatography adsorption column and DN chromatography adsorption column, to desorb and re-adsorb samarium, europium and neodymium, and collect the effluent into the waste liquid collector;

[0053] The first stage eluent of the second stage column passes through P again 204 Or HDEHP chromatography adsorption column, wash, and collect the effluent into the waste liquid collector;

[0054] The fifth stage eluent of the second column passes through P 204 Or HDEHP chromatography adsorption column, the effluent is collected into the cerium product collector to obtain the γ-radioactive solution of cerium;

[0055] The sixth stage eluent of the second stage column passes through P 204 Or HDEHP chromatography adsorption column, the effluent is collected into the terbium product collector to obtain the terbium gamma radioactive solution;

[0056] The first-stage eluent of the third-stage column passes through the BCPDTPA chromatography adsorption column, and the effluent is collected into the waste liquid collector;

[0057] The second-stage eluent of the third-stage column passes through a BCPDTPA chromatography adsorption column, and the effluent is collected into a curium product collector to obtain a radioactive curium solution;

[0058] The second-stage eluent of the third-stage column passes through the BCPDTPA chromatography adsorption column again, and the effluent is collected into the waste liquid collector;

[0059] The third-stage eluent of the third-stage column passes through the BCPDTPA chromatography adsorption column, and the effluent is collected into the americium product collector to obtain a radioactive americium solution;

[0060] The first-stage eluent of the fourth-stage column passes through the DN chromatography adsorption column, and the effluent is collected into the waste liquid collector;

[0061] The fourth stage column second stage eluent passes through the DN chromatographic adsorption column, and the effluent is collected in a samarium product collector to obtain a gamma radioactive solution of samarium;

[0062] The fourth stage column second stage eluent passes through the DN chromatographic adsorption column, and the effluent is collected in a samarium product collector to obtain a gamma radioactive solution of samarium;

[0063] The fourth stage column second stage eluent passes through the DN chromatographic adsorption column again, and the effluent is collected in a waste liquid collector.

[0064] The fourth stage column third stage eluent passes through the DN chromatographic adsorption column, and the effluent is collected in an europium product collector to obtain a gamma radioactive solution of europium.

[0065] The above separation method is used for separating isotopes of trivalent actinides and isotopes of rare earth fission fragment nuclides.

[0066] The method has the following advantages:

[0067] The method effectively utilizes the difference in chemical complexation behaviors of trivalent actinides and rare earth fission fragment nuclides on different chromatographic adsorption columns, removes interfering nuclides through RE or TRU chromatographic adsorption columns, and realizes high selectivity separation and recovery of trivalent actinides and rare earth fission fragment nuclides through elution and desorption. 204 The method effectively utilizes the difference in chemical complexation behaviors of trivalent actinides and rare earth fission fragment nuclides on different chromatographic adsorption columns, removes interfering nuclides through RE or TRU chromatographic adsorption columns, and realizes high selectivity separation and recovery of trivalent actinides and rare earth fission fragment nuclides through elution and desorption.

[0068] The method effectively utilizes the difference in chemical complexation behaviors of trivalent actinides and rare earth fission fragment nuclides on different chromatographic adsorption columns, removes interfering nuclides through RE or TRU chromatographic adsorption columns, and realizes high selectivity separation and recovery of trivalent actinides and rare earth fission fragment nuclides through elution and desorption.

[0069] The method effectively utilizes the difference in chemical complexation behaviors of trivalent actinides and rare earth fission fragment nuclides on different chromatographic adsorption columns, removes interfering nuclides through RE or TRU chromatographic adsorption columns, and realizes high selectivity separation and recovery of trivalent actinides and rare earth fission fragment nuclides through elution and desorption.

[0070] The method effectively utilizes the difference in chemical complexation behaviors of trivalent actinides and rare earth fission fragment nuclides on different chromatographic adsorption columns, removes interfering nuclides through RE or TRU chromatographic adsorption columns, and realizes high selectivity separation and recovery of trivalent actinides and rare earth fission fragment nuclides through elution and desorption. 3 The chemical recovery rates of the trivalent actinides and the rare earth fission fragment nuclides reach 85% to 97%, the decontamination factors of the trivalent actinides reach 2*10 2 , and the decontamination factors of the rare earth fission fragment nuclides reach 105 The decontamination factor for other fission products is 10 4 ~ 10 6 . BRIEF DESCRIPTION OF DRAWINGS

[0071] Figure 1 Figure 1 is a schematic diagram of the separation apparatus for Example 1 of the present application;

[0072] Figure 2 Figure 2 is a gamma-ray spectrum of the original solution containing trivalent actinides and fission products for Example 1 of the present application;

[0073] Figure 3 Figure 3 is a gamma-ray spectrum of the cerium fission product obtained from Example 1 of the present application;

[0074] Figure 4 Figure 4 is a gamma-ray spectrum of the terbium fission product obtained from Example 1 of the present application;

[0075] Figure 5 Figure 5 is a gamma-ray spectrum of the neodymium fission product obtained from Example 1 of the present application;

[0076] Figure 6 Figure 6 is a gamma-ray spectrum of the samarium fission product obtained from Example 1 of the present application;

[0077] Figure 7 Figure 7 is a gamma-ray spectrum of the europium fission product obtained from Example 1 of the present application.

[0078] The reference numerals are as follows:

[0079] 1. A reservoir for the radioactive solution containing trivalent actinides and fission products, 2. A reservoir for the washing solution, 3. A reservoir for the first stage column eluent, 4. A reservoir for the first stage eluent of the second stage column, 5. A reservoir for the second stage eluent of the second stage column, 6. A reservoir for the third stage eluent of the second stage column, 7. A reservoir for the fourth stage eluent of the second stage column, 8. A reservoir for the fifth stage eluent of the second stage column, 9. A reservoir for the sixth stage eluent of the second stage column, 10. A reservoir for the first stage eluent of the third stage column, 11. A reservoir for the second stage eluent of the third stage column, 12. A reservoir for the third stage eluent of the third stage column, 13. A reservoir for the first stage eluent of the fourth stage column, 14. A reservoir for the second stage eluent of the fourth stage column, 15. A reservoir for the third stage eluent of the fourth stage column, 16. A RE or TRU chromatographic adsorption column, 17. A P 204Or HDEHP chromatography adsorption column, 18. BCPDTPA chromatography adsorption column, 19. DN chromatography adsorption column, 20. Curium product collector, 21. Americium product collector, 22. Cerium product collector, 23. Terbium product collector, 24. Samarium product collector, 25. Europium product collector, 26. Neodymium product collector, 27. Waste liquid collector, 30. Transfer pump, 31. Valve. DETAILED DESCRIPTION

[0080] The present invention will be further described in detail below with reference to the accompanying drawings and specific embodiments.

[0081] like Figure 1 As shown, the present invention's apparatus for separating radioactive solutions of trivalent actinides and rare earth fragments includes a liquid storage tank unit, a chromatography separation unit, a waste liquid collector 27, and a product collection unit. These units and components are connected by pipelines, preferably silicone tubes. The pipelines are equipped with corresponding valves 31 and delivery pumps 30. Valve 31 is a solenoid valve, and delivery pump 30 is a peristaltic pump. This allows the solenoid valve and peristaltic pump to be controlled by a microcomputer, enabling automated control of the separation process, minimizing the impact of radioactive nuclide radiation on the human body and reducing labor intensity. The peristaltic pump delivers the separation liquid using a hose extrusion method, and the liquid flow rate and velocity are controlled by the peristaltic pump's rotational speed.

[0082] The reservoir unit includes a radioactive solution reservoir 1 containing trivalent actinides and rare earth fragment nuclides, a washing liquid reservoir 2, a first-stage column eluent reservoir 3, a second-stage column first-stage eluent reservoir 4, a second-stage column second-stage eluent reservoir 5, a second-stage column third-stage eluent reservoir 6, a second-stage column fourth-stage eluent reservoir 7, a second-stage column fifth-stage eluent reservoir 8, a second-stage column sixth-stage eluent reservoir 9, a third-stage column first-stage eluent reservoir 10, a third-stage column second-stage eluent reservoir 11, a third-stage column third-stage eluent reservoir 12, a fourth-stage column first-stage eluent reservoir 13, a fourth-stage column second-stage eluent reservoir 14, and a fourth-stage column third-stage eluent reservoir 15. Each reservoir is connected to a corresponding chromatographic adsorption column via a valve and a pump to achieve different functions.

[0083] The chromatography separation unit includes RE or TRU chromatography adsorption column 16, P 204 Or HDEHP chromatography adsorption column 17, BCPDTPA chromatography adsorption column 18, DN chromatography adsorption column 19.

[0084] The product collection unit includes a curium product collector 20, an americium product collector 21, a cerium product collector 22, a terbium product collector 23, a samarium product collector 24, a europium product collector 25, and a neodymium product collector 26;

[0085] The connection relationship between the liquid storage tank and the chromatographic column is as follows: the radioactive solution storage tank 1 containing trivalent actinide and rare earth fission fragment nuclides, the washing liquid storage tank 2, the first-stage column elution liquid storage tank 3, the second-stage column first-stage elution liquid storage tank 4, the second-stage column second-stage elution liquid storage tank 5, the second-stage column third-stage elution liquid storage tank 6, the second-stage column fourth-stage elution liquid storage tank 7, the second-stage column fifth-stage elution liquid storage tank 8, the second-stage column sixth-stage elution liquid storage tank 9, the third-stage column first-stage elution liquid storage tank 10, the third-stage column second-stage elution liquid storage tank 11, the third-stage column third-stage elution liquid storage tank 12, the fourth-stage column first-stage elution liquid storage tank 13, the fourth-stage column second-stage elution liquid storage tank 14, and the fourth-stage column third-stage elution liquid storage tank 15 are arranged side by side at the uppermost end, and the outlets of the storage tanks are connected to the corresponding inlets of the valve 31 and the delivery pump 30; the outlet of the delivery pump 30 is connected to the inlets of the RE or TRU chromatographic column 16, the P 204 or HDEHP chromatographic column 17, the BCPDTPA chromatographic column 18, and the DN chromatographic column 19 through the valve respectively; the outlet of the RE or TRU chromatographic column 16 is connected to the inlets of the P 204 or HDEHP chromatographic column 17 and the waste liquid collector 27 through the valve respectively; the outlet of the P 204 or HDEHP chromatographic column 17 is connected to the inside bottom end of the third-stage column third-stage elution liquid storage tank 10, the cerium product collector 22, the terbium product collector 23, the inlets of the DN chromatographic column 19 and the waste liquid collector 27 through the valve respectively; the outlet of the BCPDTPA chromatographic column 18 is connected to the inlets of the curium product collector 20, the americium product collector 21 and the waste liquid collector 27 through the valve respectively; and the outlet of the DN chromatographic column 19 is connected to the inlets of the samarium product collector 24, the europium product collector 25, the neodymium product collector 26 and the waste liquid collector 27 through the valve.

[0086] The separation steps of the application are as follows:

[0087] The first step is preparation before separation

[0088] The radioactive sample containing trivalent actinide and rare earth fission fragment nuclides is first dissolved in nitric acid with a concentration of 1-4 mol / L, and then sodium nitrite is added for heating at 90-100 degrees and cooling to form the radioactive sample containing trivalent actinide and rare earth fission fragment nuclides in water; the washing and elution acids are dissolved in water respectively to form the washing liquid and the elution liquid in water; the washing and elution acids are one of nitric acid and hydrochloric acid, or a mixture of diethylenetriamine pentaacetic acid and lactic acid, and the concentration of the washing and elution acids is 0.01-10 mol / L; the RE or TRU resin, the P 204 or HDEHP resin, the BCPDTPA resin and the DN resin are respectively packed into chromatographic columns.

[0089] The RE or TRU chromatographic adsorption column is mainly used to separate Am, Cm, Ce, Nd, Sm, Eu, Tb and other actinides and fission products. 204 The RE or TRU chromatographic adsorption column is mainly used to separate Am, Cm, Ce, Nd, Sm, Eu, Tb and other actinides and fission products. The BCPDTPA chromatographic adsorption column is mainly used to separate Am and Cm.

[0090] The second step: using the peristaltic pump delivery and electromagnetic valve gating mode, so that the radioactive sample containing trivalent actinides and rare earth fission nuclides is separated and adsorbed through the RE or TRU chromatographic adsorption column 16, and the effluent is collected as waste liquid.

[0091] The third step: using the peristaltic pump delivery and electromagnetic valve gating mode, so that the washing liquid is washed through the RE or TRU chromatographic adsorption column 16, and the effluent is collected as waste liquid.

[0092] The fourth step: using the peristaltic pump delivery and electromagnetic valve gating mode, so that the first-stage column eluent is sequentially eluted through the RE or TRU chromatographic adsorption column 16 and the P 204 or HDEHP chromatographic adsorption column 17, and the effluent is collected as waste liquid.

[0093] The fifth step: using the peristaltic pump delivery and electromagnetic valve gating mode, so that the second-stage column first-stage eluent is washed through the P 204 or HDEHP chromatographic adsorption column 17, and the effluent is collected as waste liquid.

[0094] The sixth step: using the peristaltic pump delivery and electromagnetic valve gating mode, so that the second-stage column second-stage eluent is eluted through the P 204 or HDEHP chromatographic adsorption column 17, and the effluent is collected in the third-stage column first-stage eluent storage tank 10.

[0095] The seventh step: using the peristaltic pump delivery and electromagnetic valve gating mode, so that the second-stage column third-stage eluent is washed through the P 204 or HDEHP chromatographic adsorption column 17, and the effluent is collected as waste liquid.

[0096] The eighth step: using the peristaltic pump delivery and electromagnetic valve gating mode, so that the second-stage column fourth-stage eluent is sequentially eluted through the P 204Alternatively, the HDEHP chromatography adsorption column 17 and the DN chromatography adsorption column 19 are used to desorb and re-adsorb samarium, europium, and neodymium, and the effluent is collected as waste liquid;

[0097] Step 9: Use the peristaltic pump to deliver and the solenoid valve to select, so that the first stage eluent of the second stage column passes through the P again. 204 Or the HDEHP chromatography adsorption column 17 is washed, and the effluent is collected as waste liquid;

[0098] Step 10: Use the peristaltic pump to deliver and the solenoid valve to select, so that the fifth stage eluent of the second stage column passes through P 204 Or HDEHP chromatography column 17; the effluent, i.e., the γ-radioactive solution of cerium, is collected in the cerium product collector 22;

[0099] Step 11: Use the peristaltic pump to deliver and the solenoid valve to select, so that the sixth stage eluent of the second stage column passes through P 204 Or HDEHP chromatography column 17; the effluent, i.e., the terbium gamma radioactive solution, is collected in the terbium product collector 23;

[0100] Step 12: Use a peristaltic pump to deliver and a solenoid valve to select, so that the first-stage eluent of the third-stage column passes through the BCPDTPA chromatography adsorption column 18, and the effluent is collected as waste liquid;

[0101] Step 13: Using a peristaltic pump and a solenoid valve, the second-stage eluent of the third-stage column passes through the BCPDTPA chromatography adsorption column 18; the effluent, i.e., the radioactive curium solution, is collected in the curium product collector 20;

[0102] Step 14: Use a peristaltic pump to deliver and a solenoid valve to select, so that the second-stage eluent of the third-stage column passes through the BCPDTPA chromatography adsorption column 18 again, and the effluent is collected as waste liquid;

[0103] Step 15: The third-stage eluent of the third-stage column passes through the BCPDTPA chromatography adsorption column 18 by using a peristaltic pump for delivery and a solenoid valve for selection; the effluent, i.e., the radioactive solution of americium, is collected in the americium product collector 21;

[0104] Step 16: Use a peristaltic pump to deliver and a solenoid valve to select, so that the first-stage eluent of the fourth-stage column passes through the DN chromatography adsorption column 19, and the effluent is collected as waste liquid;

[0105] Step 17: The second-stage eluent of the fourth-stage column is passed through the DN chromatography adsorption column 19 by using a peristaltic pump and a solenoid valve. The effluent, i.e., the neodymium gamma-radioactive solution, is collected in the neodymium product collector 26.

[0106] Step 18: The second-stage eluent of the fourth-stage column is passed through the DN chromatography adsorption column 19 by using a peristaltic pump and a solenoid valve. The effluent, i.e., the γ-radioactive solution of samarium, is collected in the samarium product collector 24.

[0107] Step 19: Use a peristaltic pump to deliver and a solenoid valve to select, so that the second-stage eluent of the fourth-stage column passes through the DN chromatography adsorption column 19 again, and the effluent is collected as waste liquid;

[0108] Step 20: Use a peristaltic pump to deliver and a solenoid valve to select, so that the third-stage eluent of the fourth-stage column passes through the DN chromatography adsorption column 19; the effluent, i.e., the γ-radioactive europium solution, is collected in the europium product collector 25.

[0109] In the above method, the trivalent actinide elements are various isotopes including americium and curium, and the rare earth fragment nuclides are various isotopes including cerium, neodymium, samarium, europium, and terbium.

[0110] Example 1

[0111] Dissolve the radioactive sample containing trivalent actinides and rare earth fragments in 10mL 2mol / L HNO3, add sodium nitrite and heat at 90-100 degrees, and cool to form a solution containing trivalent actinides and rare earth fragments. Place the solution in the liquid storage tank 1. The γ-radiation spectrum is as follows: Figure 2 shown.

[0112] The flow rate of the solution containing trivalent actinides and rare earth fragments is controlled at 1 mL / min, so that the radioactive sample containing trivalent actinides and rare earth fragments is separated and adsorbed by the RE or TRU chromatographic adsorption column 16, wherein the RE or TRU chromatographic adsorption column 16 is An RE or TRU chromatography adsorption column is used to separate Am, Cm, Ce, Nd, Sm, Eu, Tb from Tc, Te, I, Ba, Ru, Rh, Nb, etc., and the effluent is collected in a waste liquid collector 27.

[0113] Use 25 mL of 2 mol / L HNO3 solution in the washing liquid reservoir 2, control the flow rate at 1.5 mL / min, and wash through the RE or TRU chromatography adsorption column 16 to achieve further separation of Mo and Tc, Te, I, Ba, Ru, Rh, Nb, etc., and collect the effluent in the waste liquid collector 27.

[0114] Use 25mL of 0.05mol / L HNO3 solution in the first column eluent reservoir 3, control the flow rate at 1.0mL / min, and pass it through the RE or TRU chromatography adsorption column 16 and P 204 Or HDEHP chromatography adsorption column 17 for elution, wherein P 204 Or HDEHP chromatography adsorption column 17 is P 204 or HDEHP chromatographic adsorption column 17, to realize the desorption and re-adsorption of trivalent actinides and rare earth fission products, and the effluent is collected in waste liquid collector 27.

[0115] Use 25 mL of 0.1 mol / L HNO3 solution in the second-stage column first-stage elution liquid storage tank 4, control the flow rate at 1.0 mL / min, pass through P 204 or HDEHP chromatographic adsorption column 17, to realize the desorption and re-adsorption of trivalent actinides and rare earth fission products, and the effluent is collected in waste liquid collector 27.

[0116] Use 30 mL of 0.05 mol / L DTPA-1 mol / L lactic acid (pH 3.0) solution in the second-stage column second-stage elution liquid storage tank 5, control the flow rate at 1.0 mL / min, pass through P 204 or HDEHP chromatographic adsorption column 17, to realize the desorption and re-adsorption of trivalent actinides and rare earth fission products, and the effluent is collected in waste liquid collector 27.

[0117] Use 40 mL of 0.2 mol / L HNO3-0.07 mol / L NaBrO3 solution in the second-stage column third-stage elution liquid storage tank 6, control the flow rate at 1.0 mL / min, pass through P 204 or HDEHP chromatographic adsorption column 17, to realize the desorption and re-adsorption of trivalent actinides and rare earth fission products, and the effluent is collected in waste liquid collector 27.

[0118] Use 20 mL of 1 mol / L HNO3-0.07 mol / L NaBrO3 solution in the second-stage column fourth-stage elution liquid storage tank 7, control the flow rate at 1.0 mL / min, pass through P 204 or HDEHP chromatographic adsorption column 17, to realize the desorption and re-adsorption of trivalent actinides and rare earth fission products, and the effluent is collected in waste liquid collector 27. DN chromatographic adsorption column, to realize the desorption and re-adsorption of samarium, europium and neodymium, and the effluent is collected in waste liquid collector 27.

[0119] Use 20 mL of 0.1 mol / L HNO3 solution in the second-stage column first-stage elution liquid storage tank 4, control the flow rate at 1.0 mL / min, pass through P 204 or HDEHP chromatographic adsorption column 17, to realize the desorption and re-adsorption of trivalent actinides and rare earth fission products, and the effluent is collected in waste liquid collector 27.

[0120] Use 15 mL of 1 mol / L HNO3 solution in the second-stage column fifth-stage elution liquid storage tank 8, control the flow rate at 1.0 mL / min, pass through P 204 or HDEHP chromatographic adsorption column 17, and the effluent is collected in cerium product collector 22, which is the gamma radioactivity measurement source of cerium.

[0121] Use 15mL 3mol / L HNO3 solution from the sixth stage eluent reservoir 9 of the second stage column, control the flow rate to 0.5mL / min, and pass through P 204 Or HDEHP chromatography adsorption column 17, the effluent is collected in the terbium product collector 23, which is the γ radioactive measurement source of terbium.

[0122] 31.2 mL of 0.05 mol / L DTPA-1 mol / L lactic acid solution in the first eluent reservoir 10 of the third column was used to control the flow rate to 1.0 mL / min and pass through the BCPDTPA chromatography adsorption column 18, wherein the BCPDTPA chromatography adsorption column 18 is The BCPDTPA chromatography adsorption column is used, and the effluent is collected in the waste liquid collector 27.

[0123] Use 15 mL of 0.1 mol / L HNO3 solution in the second-stage eluent reservoir 11 of the third-stage column, control the flow rate at 1.0 mL / min, and pass it through the BCPDTPA chromatography adsorption column 18; the effluent, i.e., the γ-radioactive solution of curium, is collected in the curium product collector 20.

[0124] Use 15 mL of 0.1 mol / L HNO3 solution in the second-stage eluent reservoir 11 of the third-stage column, control the flow rate at 1.0 mL / min, and elute again through the BCPDTPA chromatography adsorption column 18, and collect the effluent in the waste liquid collector 27.

[0125] 8 mL of 1 mol / L HNO3 solution in the third-stage eluent reservoir 12 of the third-stage column is used to control the flow rate to 1.0 mL / min and pass through the BCPDTPA chromatography adsorption column 18; the effluent, i.e., the radioactive solution of americium, is collected in the americium product collector 21.

[0126] Use 40 mL of 2.75 mol / L HCl solution in the first-stage eluent reservoir 13 of the fourth-stage column, control the flow rate to 1.0 mL / min, and pass it through the DN chromatography adsorption column 19 at the same time. The effluent is collected in the waste liquid collector 27.

[0127] Use 15mL of 1.5mol / L HCl solution in the second-stage eluent reservoir 14 of the fourth-stage column, control the flow rate to 0.5mL / min, pass through the DN chromatography adsorption column 19, and collect the effluent in the neodymium product collector 27, which is the measurement source of neodymium γ radioactivity.

[0128] Use 10 mL of 1.5 mol / L HCl solution in the second-stage eluent reservoir 14 of the fourth-stage column, control the flow rate to 0.5 mL / min, pass through the DN chromatography adsorption column 19, and collect the effluent in the samarium product collector 24, which is the measurement source of the γ radioactivity of samarium.

[0129] Use 10 mL of 1.5 mol / L HCl solution in the second-stage eluent reservoir 14 of the fourth-stage column, control the flow rate to 0.5 mL / min, and pass it through the DN chromatography adsorption column 19 again. The effluent is collected in the waste liquid collector 27.

[0130] Use 10 mL of 0.1 mol / L HCl solution in the third-stage eluent reservoir 15 of the fourth-stage column, control the flow rate to 0.5 mL / min, pass through the DN chromatography adsorption column 19, and collect the effluent in the europium product collector 25, which is the measurement source of europium γ radioactivity.

[0131] The experimentally obtained γ-radiation energy spectra of cerium, terbium, neodymium, samarium and europium are as follows: Figure 3 、 Figure 4 、 Figure 5 、 Figure 6 、 Figure 7 The recovery rates of americium, curium, cerium, neodymium, samarium, europium, and terbium were 92.6%, 91.2%, 96.2%, 94.4%, 85.7%, 89.3%, and 95.9%, respectively. The decontamination factor between americium and curium was 2×10 3 The decontamination factors of cerium, neodymium, samarium, europium and terbium are within 10 2 ~10 5 The decontamination factor for other fission products is 10 4 ~10 6 .

[0132] Example 2

[0133] The RE chromatography adsorption column in Example 1 was replaced with a TRU chromatography adsorption column. 204 The chromatographic adsorption column was replaced with a HDEHP chromatographic adsorption column, and the separation process of Example 1 was repeated to obtain radioactive measurement sources of americium, curium, cerium, neodymium, samarium, europium, and terbium. The recoveries were 93.3%, 90.1%, 96.9%, 95.3%, 85.2%, 88.4%, and 93.4%, respectively. The decontamination factors are shown in Tables 1 and 2. It can be seen that the decontamination factor between americium and curium is as high as 2×10 3 The decontamination factor between rare earth fragment nuclides is 10 2 ~10 5 The decontamination factor for other fission products is 10 4 ~10 6 .

[0134] Table 1 Analysis of recovery rate and decontamination factor of americium and curium

[0135]

[0136] Table 2 Analysis of the recovery rate and decontamination factor of rare earth fragments

[0137]

[0138]

[0139] Note: “>” indicates the lower limit was assigned because it was not detected.

Claims

1. A device for separating trivalent actinides and rare earth fragment nuclides, characterized in that: It includes a liquid storage tank unit, a chromatography separation unit, a waste liquid collector (27), a product collection unit, and a delivery pump (30); The liquid in the liquid storage tank unit enters the chromatography separation unit through the delivery pump (30), and the liquid flowing out of the chromatography separation unit enters the waste liquid collector (27) or the product collection unit; The liquid storage tank unit, the chromatography separation unit, the product collection unit, and the waste liquid collector (27) are connected through a pipeline, and a valve (31) is provided on the pipeline through which the liquid flows; The liquid storage tank unit is located at the uppermost end, and the waste liquid collector (27) and the product collection unit are located at the lowermost end; The liquid storage tank unit comprises a radioactive solution storage tank (1) containing trivalent actinide elements and rare earth fragment nuclides, a washing liquid storage tank (2), a first-stage column eluent storage tank (3), a second-stage column first-stage eluent storage tank (4), a second-stage column second-stage eluent storage tank (5), a second-stage column third-stage eluent storage tank (6), a second-stage column fourth-stage eluent storage tank (7), a second-stage column fifth-stage eluent storage tank (8), a second-stage column sixth-stage eluent storage tank (9), a third-stage column first-stage eluent storage tank (10), a third-stage column second-stage eluent storage tank (11), a third-stage column third-stage eluent storage tank (12), a fourth-stage column first-stage eluent storage tank (13), a fourth-stage column second-stage eluent storage tank (14), and a fourth-stage column third-stage eluent storage tank (15), all of which are located on the same horizontal plane. The chromatographic separation unit comprises a RE or TRU chromatographic adsorption column (16), a P 204 or a HDEHP chromatography adsorption column (17), a DN chromatography adsorption column (19), and a BCPDTPA chromatography adsorption column (18); P 204 Or the lower end of the HDEHP chromatography adsorption column (17) is connected to the third column first stage eluent storage tank (10) through a pipeline, P 204 Or the effluent of the HDEHP chromatography adsorption column (17) can flow to the first-stage eluent storage tank (10) of the third-stage column; The product collection unit comprises a curium product collector (20), an americium product collector (21), a cerium product collector (22), a terbium product collector (23), a samarium product collector (24), a europium product collector (25), and a neodymium product collector (26) located on the same horizontal plane; and a waste liquid collector (27) and the chromatography separation unit are located on the same horizontal plane.

2. The separation device according to claim 1, characterized in that: The valve (31) is a solenoid valve, the delivery pump (30) is a peristaltic pump, and the pipeline is a silicone tube.

3. The separation device according to claim 2, characterized in that: The utility model further comprises a microcomputer, and the microcomputer is used for controlling the electromagnetic valve and the peristaltic pump.

4. The separation device according to claim 1, characterized in that: The connection relationship between the liquid storage tank unit, the chromatography separation unit, the waste liquid collector (27), and the product collection unit is as follows: A radioactive solution storage tank containing trivalent actinides and rare earth fragment nuclides (1), a washing solution storage tank (2), a first-stage column eluent storage tank (3), a second-stage column first-stage eluent storage tank (4), a second-stage column second-stage eluent storage tank (5), a second-stage column third-stage eluent storage tank (6), a second-stage column fourth-stage eluent storage tank (7), a second-stage column fifth-stage eluent storage tank (8), a second-stage column sixth-stage eluent storage tank (9), a third-stage column first-stage eluent storage tank The outlets of the liquid storage tank (10), the second-stage eluent storage tank (11) of the third column, the third-stage eluent storage tank (12), the first-stage eluent storage tank (13) of the fourth column, the second-stage eluent storage tank (14) of the fourth column, and the third-stage eluent storage tank (15) of the fourth column are connected to the corresponding inlets of the delivery pump (30) through the valve (31); the outlet of the delivery pump (30) is connected to the RE or TRU chromatography adsorption column (16), the P 204 or HDEHP chromatography adsorption column (17), BCPDTPA chromatography adsorption column (18), DN chromatography adsorption column (19) are connected to the feed port; RE or TRU chromatography adsorption column (16) outlet is connected to P through valve (31) respectively. 204 Or the feed port of the HDEHP chromatography adsorption column (17) is connected to the waste liquid collector (27); P 204 Or the discharge port of the HDEHP chromatography adsorption column (17) is respectively connected to the inner bottom end of the third-stage column third-stage eluent storage tank (10), the cerium product collector (22), the terbium product collector (23), the feed port of the DN chromatography adsorption column (19) and the waste liquid collector (27) through a valve (31); the discharge port of the BCPDTPA chromatography adsorption column (18) is respectively connected to the curium product collector (20), the americium product collector (21) and the waste liquid collector (27) through a valve (31); and the discharge port of the DN chromatography adsorption column (19) is connected to the samarium product collector (24), the europium product collector (25), the neodymium product collector (26) and the waste liquid collector (27) through a valve (31).

5. A method for separating trivalent actinides and rare earth fragment nuclides, using any separation device according to claims 1 to 4, characterized in that: The following steps are included: Step 1, preparation before separation: The radioactive sample containing trivalent actinides and rare earth fragments to be separated is dissolved in nitric acid, sodium nitrite is added, and the mixture is heated at 90 to 100° C. and then cooled to obtain an aqueous radioactive sample containing trivalent actinides and rare earth fragments; The washing and rinsing acids are dissolved in water to obtain an aqueous washing solution and an aqueous rinsing solution respectively; the washing and rinsing acids are selected from nitric acid, hydrochloric acid, or a mixture of diethylenetriaminepentaacetic acid and lactic acid; RE or TRU resin, P 204 Or HDEHP resin, BCPDTPA resin, DN resin are respectively loaded into chromatography adsorption column to obtain RE or TRU chromatography adsorption column (16), P 204 or a HDEHP chromatography adsorption column (17), a BCPDTPA chromatography adsorption column (18), or a DN chromatography adsorption column (19); Step 2, adsorption of trivalent actinides and rare earth fragments: The aqueous radioactive sample containing trivalent actinides and rare earth fragment nuclides prepared in step 1 is placed in a radioactive solution storage tank (1) containing trivalent actinides and rare earth fragment nuclides, and the aqueous radioactive sample containing actinides and lanthanide fission products is separated and adsorbed using a RE or TRU chromatographic adsorption column (16), wherein the trivalent actinides and rare earth fragment nuclides are adsorbed in the RE or TRU chromatographic adsorption column (16), and the effluent is collected in a waste liquid collector (27); Step 3, washing: Using an aqueous washing solution, the RE or TRU chromatography adsorption column (16) is washed, and the effluent is collected into a waste liquid collector (27); Step 4, rinse: Use aqueous eluent to wash the RE or TRU chromatography column (16), P 204 Or HDEHP chromatography adsorption column (17), DN chromatography adsorption column (19), and BCPDTPA chromatography adsorption column (18) are used for elution to obtain γ-radioactive solution of cerium, γ-radioactive solution of terbium, γ-radioactive solution of americium, γ-radioactive solution of curium, γ-radioactive solution of neodymium, γ-radioactive solution of samarium, and γ-radioactive solution of europium.

6. The separation method according to claim 5, characterized in that In the preparation before separation in step 1, the concentration of nitric acid used to dissolve the radioactive sample of trivalent actinides and rare earth fragments to be separated is 1 mol / L to 4 mol / L, and the concentration of the acid used for washing and eluting is 0.01 to 10 mol / L.

7. The separation method according to claim 5, characterized in that In the preparation before separation in step 1, the aqueous washing liquid is a 1 mol / L to 4 mol / L HNO3 solution, and the aqueous washing liquid is placed in the washing liquid storage tank (2).

8. The separation method according to claim 5, characterized in that In the preparation before separation in step 1, the aqueous eluent includes the eluent of the first column, the first eluent of the second column, the second eluent of the second column, the third eluent of the second column, the fourth eluent of the second column, the fifth eluent of the second column, the sixth eluent of the second column, the first eluent of the third column, the second eluent of the third column, the third eluent of the third column, the first eluent of the fourth column, the second eluent of the fourth column, and the third eluent of the fourth column, and the above eluents are placed in corresponding liquid storage tanks; The first column eluent was 0.05 mol / L HNO3 solution at a flow rate of 1.0 mL / min; The first-stage eluent of the second-stage column is 0.1 mol / L HNO3 solution with a flow rate of 1.0 mL / min; The second-stage eluent of the second-stage column was 0.05 mol / L DTPA-1 mol / L lactic acid solution, pH 3.0, with a flow rate of 1.0 mL / min; The third eluent of the second column was 0.2 mol / L HNO3-0.07 mol / L NaBrO3 solution at a flow rate of 1.0 mL / min; the fourth eluent of the second column was 1 mol / L HNO3-0.07 mol / L NaBrO3 solution at a flow rate of 1.0 mL / min; the fifth eluent of the second column was 1 mol / L HNO3 solution at a flow rate of 1.0 mL / min; The sixth stage eluent of the second stage column is 3 mol / L HNO3 solution with a flow rate of 0.5 mL / min; The first eluent of the third column was 0.05 mol / L DTPA-1 mol / L lactic acid solution at a flow rate of 1.0 mL / min; the second eluent of the third column was 0.1 mol / L HNO3 solution at a flow rate of 1.0 mL / min; The third-stage eluent of the third-stage column is 1 mol / L HNO3 solution with a flow rate of 1.0 mL / min; The first-stage eluent of the fourth-stage column was 2.75 mol / L HCl solution with a flow rate of 1.0 mL / min; The second-stage eluent of the fourth-stage column was 1.5 mol / L HCl solution with a flow rate of 0.5 mL / min; The third-stage eluent of the fourth-stage column is 0.1 mol / L HCl solution, and the flow rate is 0.5 mL / min.

9. The separation method according to claim 5, characterized in that The step 4 of eluting further comprises: The first column eluent passes through the RE or TRU chromatography adsorption column (16) and P 204 or HDEHP chromatography adsorption column (17), to desorb and re-adsorb trivalent actinides and rare earth fragment nuclides, and the effluent is collected in a waste liquid collector (27); The first stage eluent of the second stage column passes through P 204 or HDEHP chromatography adsorption column (17), washing, and collecting the effluent into the waste liquid collector (27); The second stage eluent of the second stage column passes through P 204 or HDEHP chromatography adsorption column (17) to desorb trivalent actinides, and the effluent is collected into the first-stage eluent storage tank (10) of the third-stage column; The second column and the third stage eluent pass through P 204 or HDEHP chromatography adsorption column (17), washing, and collecting the effluent into the waste liquid collector (27); The second column and the fourth stage eluent pass through P 204 or HDEHP chromatography adsorption column (17) and DN chromatography adsorption column (19), to desorb and re-adsorb samarium, europium and neodymium, and collect the effluent into a waste liquid collector (27); The first stage eluent of the second stage column passes through P again 204 or HDEHP chromatography adsorption column (17), washing, and collecting the effluent into the waste liquid collector (27); The fifth stage eluent of the second column passes through P 204 or HDEHP chromatography adsorption column (17), the effluent is collected into a cerium product collector (22), and a γ-radioactive solution of cerium is obtained; The sixth stage eluent of the second stage column passes through P 204 or HDEHP chromatography adsorption column (17), the effluent is collected into a terbium product collector (23), and a terbium gamma radioactive solution is obtained; The first-stage eluent of the third-stage column passes through the BCPDTPA chromatography adsorption column (18), and the effluent is collected in the waste liquid collector (27); The second-stage eluent of the third-stage column passes through a BCPDTPA chromatography adsorption column (18), and the effluent is collected in a curium product collector (20) to obtain a radioactive curium solution; The second-stage eluent of the third-stage column passes through the BCPDTPA chromatography adsorption column (18) again, and the effluent is collected in the waste liquid collector (27); The third-stage eluent of the third-stage column passes through a BCPDTPA chromatography adsorption column (18), and the effluent is collected in an americium product collector (21) to obtain a radioactive americium solution; The first-stage eluent of the fourth-stage column passes through the DN chromatography adsorption column (19), and the effluent is collected in the waste liquid collector (27); The second-stage eluent of the fourth-stage column passes through the DN chromatography adsorption column (19), and the effluent is collected in the neodymium product collector (26) to obtain a neodymium gamma radioactive solution; The second-stage eluent of the fourth-stage column passes through the DN chromatography adsorption column (19), and the effluent is collected in the samarium product collector (24) to obtain a samarium γ-radioactive solution; The second-stage eluent of the fourth-stage column passes through the DN chromatography adsorption column (19) again, and the effluent is collected in the waste liquid collector (27); The third-stage eluent of the fourth-stage column passes through a DN chromatography adsorption column (19), and the effluent is collected in a europium product collector (25) to obtain a europium gamma radioactive solution.

10. The separation method according to claim 5, characterized in that: Trivalent actinides are isotopes of americium and curium, and rare earth fragment nuclides are isotopes of cerium, neodymium, samarium, europium, and terbium.

Images