Separation device and separation method for trivalent actinide elements and rare earth splinter nuclides

Abstract

The invention relates to a separation device and a separation method for trivalent actinide elements and rare earth fission nuclides, belongs to the technical field of separation of actinide elements and fission products, and solves the technical problems of low decontamination and low recovery rate in separation. The separation device comprises a liquid storage tank unit, a color layer separation unit, a waste liquid collector, a product collection unit 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 collection unit. The liquid storage tank unit, the color layer separation unit, the product collection unit and the waste liquid collector are communicated through a pipeline, and a valve is arranged on the pipeline. The separation method comprises the following steps: preparation before separation, adsorption of trivalent actinide elements and rare earth splinter nuclides, washing and leaching. The method is used for separating the trivalent actinide elements and the rare earth splinter nuclides.

Description

Technical Field

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

[0002] The radiochemical analysis of activation products and fission products in the spent fuel solution can determine the reactor burnup and neutron flux. The plutonium isotope Pu-241 has a half-life of 14.29 years. It undergoes radioactive decay to produce the daughter Am-241 with a half-life of 432.2 years. Under the action of neutrons, it undergoes an activation reaction to produce the decay product Cm-242 (half-life 163 days). By analyzing and measuring the americium curium isotope, information such as neutron flux can be obtained. Fissionable 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, which are 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 high yield (5.98%), becoming the fission product of key concern in reactor burnup monitoring analysis and fission yield determination.

[0003] The measurement of americium and curium isotopes usually adopts semiconductor α-spectroscopy and mass spectrometry. However, due to the relatively low energy resolution of semiconductor α-spectrometer, the Cm-242 energy spectrum peak 6.113MeV causes strong peak tailing interference to the Am-241 energy spectrum peak 5.485MeV; there is isotopic interference of Cm-242 in the mass spectrometry measurement of Am-242m. In order to achieve accurate measurement and analysis of americium and curium isotopes, it is necessary to solve the problem of mutual separation between americium and curium isotopes. The γ-radioactive fission products of rare earth fragment nuclides Ce-141, Ce-144, Nd-147, Sm-153, Eu-155, Eu-156, Tb-161, etc., each nuclide will produce multiple γ-rays, and there are different degrees of repeated peaks and cross-peak interferences in the activity measurement of the trap-type high-purity germanium γ-spectrometer. In addition, the uranium-plutonium fission process also produces a large number of other fission products with rich gamma rays, such as Mo-99, Tc-99m, Te-132, Ru-103, I-131, I-132, Ba-140, La-140, Zr-95, Nb-95, etc., which lead to serious interference of Compton plateau and spectrum peak, affecting the accurate measurement of low-activity nuclides. Therefore, it is necessary to separate and prepare radiochemically pure rare earth fragment nuclide measurement sources for analysis and determination.

[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 a method of using mixed bed (Dionex CS5A) ion chromatography to simultaneously separate and purify actinide elements uranium, plutonium, americium and lanthanide fission products (cerium, neodymium, samarium, europium, etc.) from spent fuel samples, and determined their contents by isotope dilution mass spectrometry. However, this separation method can only meet the measurement of stable lanthanide fission products (Ce-140, Nd-143, Nd-146, Sm-150, Eu-153, etc.), and failed to solve the problem of separating γ-radioactive lanthanide fission products from other interfering nuclides, nor did it involve the separation of americium and 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 rare earth element europium from acidic solution using multiple centrifugal extractors through a liquid-liquid extraction process of 7-stage extraction, 9-stage washing and 8-stage stripping. However, the separation problem of other rare earth fragments was not mentioned, and the method required expensive experimental equipment and complicated process, and was not suitable for the analysis of laboratory samples.

[0006] Arrigo et al. reported the use of UTEVA-TRU-LN resin chromatography to separate and extract γ-radioactive lanthanide fission products (Ce-144, Sm-153, Eu-156, Tb-161, etc.) from mixed fission products of uranium irradiation in Separation of lanthanide isotopes from mixed fission product samples. Separations., 2021, 8:104-114 for their cumulative fission yield measurement. However, the recovery rate of low-yield nuclide Eu-156 was not high (56%), and the decontamination factor for high-yield nuclide Nd-147 was less than 3.8×10 3 The separation and decontamination of lanthanide fission products from each other and other fission products is not thorough enough, resulting in a large uncertainty in yield determination (10.9% to 22.7%). This method cannot meet the technical requirements for high-precision testing and 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 actinide elements and rare earth fragment nuclides, the present invention provides a separation device and a separation method for trivalent actinide elements 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 chromatographic separation unit, a waste liquid collector, a product collection unit and a delivery pump.

[0010] The liquid in the liquid storage tank unit enters the chromatographic separation unit through the delivery pump, and the liquid flowing out of the chromatographic separation unit enters 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 through 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 storage tank unit includes a radioactive solution storage tank containing trivalent actinide elements and rare earth fragment nuclides, a washing liquid storage tank, a first-level column eluent storage tank, a second-level column first-level eluent storage tank, a second-level column second-level eluent storage tank, a second-level column third-level eluent storage tank, a second-level column fourth-level eluent storage tank, a second-level column fifth-level eluent storage tank, a second-level column sixth-level eluent storage tank, a third-level column first-level eluent storage tank, a third-level column second-level eluent storage tank, a third-level column third-level eluent storage tank, a fourth-level column first-level eluent storage tank, a fourth-level column second-level eluent storage tank, and a fourth-level column third-level eluent storage tank, all of which are located on the same horizontal plane.

[0014] The chromatographic separation unit includes RE or TRU chromatographic adsorption columns, P 204 Or HDEHP chromatography adsorption column, DN chromatography adsorption column, and BCPDTPA chromatography adsorption column. 204 Or the lower end of the HDEHP chromatography adsorption column is connected to the first-stage eluent storage tank of the third-stage column through a pipeline, P 204 Or the effluent from the HDEHP chromatography adsorption column can flow to the first-stage eluent reservoir of the third-stage column.

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

[0016] In the above separation device, the valve is a solenoid valve, the delivery pump is a peristaltic pump, and the pipeline is a silicone tube.

[0017] The above separation device also includes a microcomputer, which is used to control the solenoid valve and the peristaltic pump.

[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 actinide elements and rare earth fragment nuclides, the washing solution 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 inlet of the delivery pump through valves; the outlet of the delivery pump is respectively connected to the RE or TRU chromatographic adsorption column, P through valves. 204 or HDEHP chromatography adsorption column, BCPDTPA chromatography adsorption column, DN chromatography adsorption column inlet; RE or TRU chromatography adsorption column outlet through the valve and P 204 Or connect the feed port of HDEHP chromatography adsorption column to the waste liquid collector; 204 Or the discharge port of the HDEHP chromatography adsorption column is connected to the inner bottom 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 inlet 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 Isolation

[0022] The radioactive sample containing trivalent actinide elements and rare earth fragment nuclides to be separated is dissolved in nitric acid, sodium nitrite is added, and the mixture is heated and cooled at a temperature of 90 to 100° C. to obtain an aqueous radioactive sample containing trivalent actinide elements and rare earth fragment nuclides;

[0023] The washing and eluting acids are dissolved in water respectively to obtain an aqueous washing liquid and an aqueous eluting liquid; the washing and eluting acids are one of nitric acid and 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 the 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 fragment nuclides prepared in step 1 is placed in a storage tank for radioactive solution containing trivalent actinides and rare earth fragment nuclides, and an RE or TRU chromatographic adsorption column is used to separate and adsorb the aqueous radioactive sample containing actinides and lanthanide fission products, and the trivalent actinides and rare earth fragment nuclides are adsorbed in the RE or TRU chromatographic adsorption column, and the effluent is collected in a waste liquid collector;

[0027] Step 3, Washing

[0028] Use aqueous washing liquid 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 adsorb RE or TRU chromatography columns, 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 actinide elements and rare earth fragment nuclides 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 1 mol / L to 4 mol / L HNO 3 Solution, aqueous detergent is placed in the detergent reservoir.

[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 is 0.05 mol / L HNO 3 solution, flow rate 1.0 mL / min;

[0035] The first eluent of the second column is 0.1 mol / L HNO 3 solution, flow rate 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, and the flow rate was 1.0 mL / min;

[0037] The third eluent of the second column is 0.2 mol / L HNO 3 -0.07mol / L NaBrO 3 solution, flow rate 1.0 mL / min;

[0038] The fourth eluent of the second column is 1 mol / L HNO 3 -0.07mol / LNaBrO 3 solution, flow rate 1.0 mL / min;

[0039] The fifth eluent of the second column is 1 mol / L HNO 3 solution, flow rate 1.0 mL / min;

[0040] The sixth eluent of the second column is 3 mol / L HNO 3 solution, flow rate 0.5 mL / min;

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

[0042] The second eluent of the third column is 0.1 mol / L HNO 3 solution, flow rate 1.0 mL / min;

[0043] The third column eluent is 1 mol / L HNO 3 solution, flow rate 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, elution, further comprises:

[0048] The first column eluent passes through RE or TRU chromatography adsorption column and P 204 Or HDEHP chromatography adsorption column, desorption and re-adsorption of trivalent actinide elements and rare earth fragment nuclides, and the effluent is collected in a 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 column second stage eluent 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 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 eluent pass through P 204 Or HDEHP chromatography adsorption column and DN chromatography adsorption column, desorption and re-adsorption of samarium, europium and neodymium, and the effluent is collected in a 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 column passes through P 204 Or HDEHP chromatography adsorption column, the effluent is collected into a terbium product collector to obtain a 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 in the waste liquid collector;

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

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

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

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

[0063] The second-stage eluent of the fourth-stage column passes through the DN chromatography adsorption column again, and the effluent is collected in the waste liquid collector;

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

[0065] In the above separation method, the trivalent actinide elements are isotopes of americium and curium, and the rare earth fragment nuclides are isotopes of cerium, neodymium, samarium, europium and terbium.

[0066] The beneficial effects of the present invention are:

[0067] A method for separating trivalent actinide elements and rare earth fragment nuclides, which effectively utilizes the difference in chemical complexation behavior between trivalent actinide elements americium curium and rare earth fragment nuclides cerium, neodymium, samarium, europium and terbium on different chromatographic adsorption columns, removes interfering nuclides through RE or TRU chromatographic adsorption columns, and makes americium curium adsorbed on BCPDTPA chromatographic columns, cerium and terbium adsorbed on P 204 Or HDEHP chromatography adsorption column, neodymium, samarium and europium are adsorbed on the DN chromatography column, and through elution and desorption, the three actinide elements such as americium, curium, cerium, neodymium, samarium, europium and terbium and rare earth fragment nuclides are separated and recovered with high selectivity.

[0068] A separation method for trivalent actinide elements and rare earth fragment nuclides, with clear separation unit functions, ingenious dynamic transformation and connection of inter-column media, and easy flow rate control. A streamlined automatic control separation process of synchronous adsorption, elution, and desorption is constructed using a simple four-stage separation unit.

[0069] A method for separating trivalent actinide elements and rare earth fragment nuclides. The entire separation process from the absorption of original radioactive liquid to the preparation of trivalent actinide elements americium curium and rare earth fragment nuclides cerium, neodymium, samarium, europium and terbium radioactive measurement sources is automatically controlled by a microcomputer program, which can significantly reduce the radiation dose of operators.

[0070] A method for separating trivalent actinide elements and rare earth fragment nuclides. Compared with the existing method, the method realizes the synchronous and efficient separation of trivalent actinide elements americium and curium and rare earth fragment nuclides cerium, neodymium, samarium, europium and terbium under automatic control conditions; the chemical recovery rate of americium, curium, cerium, neodymium, samarium, europium and terbium reaches 85% to 97%, and the decontamination factor between americium and curium reaches 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 . BRIEF DESCRIPTION OF THE DRAWINGS

[0071] Figure 1 This is a schematic diagram of a separation device according to Example 1 of the present invention;

[0072] Figure 2 The γ-radiation spectrum of the original solution containing trivalent actinide elements and rare earth fragment nuclides used in Example 1 of the present invention;

[0073] Figure 3 This is the γ-radioactivity spectrum of the rare earth fragment nuclide cerium separated in Example 1 of the present invention;

[0074] Figure 4 This is the γ-radioactivity spectrum of the rare earth fragment nuclide terbium separated in Example 1 of the present invention;

[0075] Figure 5 This is the radioactivity spectrum of neodymium gamma nuclide of rare earth fragments separated in Example 1 of the present invention;

[0076] Figure 6 The radioactivity spectrum of the rare earth fragment nuclide samarium gamma obtained by separation in Example 1 of the present invention;

[0077] Figure 7 This is the radioactivity spectrum of europium gamma radionuclides of rare earth fragments separated in Example 1 of the present invention.

[0078] The reference numerals are as follows:

[0079] 1. A reservoir for radioactive solution containing trivalent actinide elements and rare earth fragment nuclides, 2. A reservoir for washing solution, 3. A reservoir for eluent of the first column, 4. A reservoir for eluent of the first column, 5. A reservoir for eluent of the second column, 6. A reservoir for eluent of the third column, 7. A reservoir for eluent of the fourth column, 8. A reservoir for eluent of the fifth column, 9. A reservoir for eluent of the sixth column, 10. A reservoir for eluent of the first column, 11. A reservoir for eluent of the second column, 12. A reservoir for eluent of the third column, 13. A reservoir for eluent of the first column, 14. A reservoir for eluent of the second column, 15. A reservoir for eluent of the third column, 16. A RE or TRU chromatography adsorption column, 17. P 204 Or 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. delivery pump, 31. valve. DETAILED DESCRIPTION

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

[0081] like Figure 1 As shown, the separation device of the radioactive solution of trivalent actinide elements and rare earth fragment nuclides of the present invention includes a liquid storage tank unit, a chromatographic separation unit, a waste liquid collector 27, and a product collection unit. The above units and devices are connected by pipelines. Preferably, the pipeline adopts a silicone tube; and a corresponding valve 31 and a delivery pump 30 are configured in the pipeline. The valve 31 is a solenoid valve, and the delivery pump 30 is a peristaltic pump. In this way, the solenoid valve and the peristaltic pump can be controlled by a microcomputer to realize automatic control of the separation process, reduce the impact of radioactive nuclides 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.

[0082] 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. Each storage tank is connected to a corresponding chromatographic adsorption column through a valve and a pump to realize different functions.

[0083] The chromatographic separation unit includes an RE or TRU chromatographic adsorption column 16, a 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 reservoir and the chromatographic adsorption column is as follows: a radioactive solution reservoir 1 containing trivalent actinide elements 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 The first eluent reservoir 10, the second eluent reservoir 11 of the third column, the third eluent reservoir 12 of the third column, the first eluent reservoir 13 of the fourth column, the second eluent reservoir 14 of the fourth column, and the third eluent reservoir 15 of the fourth column are arranged in parallel at the top, and the outlet of each reservoir is connected to the corresponding inlet of the delivery pump 30 through a valve 31; the outlet of the delivery pump 30 is connected to the RE or TRU chromatography adsorption column 16, P through a valve. 204 or the feed inlet of the HDEHP chromatography adsorption column 17, the BCPDTPA chromatography adsorption column 18, and the DN chromatography adsorption column 19; the discharge port of the RE or TRU chromatography adsorption column 16 is connected to the P through the valve 31 respectively. 204 Or the feed port of the HDEHP chromatography adsorption column 17 is connected to the waste liquid collector 27; 204Or the discharge port of the HDEHP chromatography adsorption column 17 is connected to the inner bottom end of the third column third 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 the valve 31; the discharge port of the BCPDTPA chromatography adsorption column 18 is connected to the curium product collector 20, the americium product collector 21 and the waste liquid collector 27 through the valve 31; 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 the valve 31.

[0086] The separation step of the present invention is:

[0087] Step 1: Preparation before separation

[0088] The radioactive sample containing trivalent actinides and rare earth fragment nuclides is first dissolved in nitric acid with a concentration of 1 to 4 mol / L, and then sodium nitrite is added to heat at 90 to 100 degrees and then cooled to form an aqueous radioactive sample containing trivalent actinides and rare earth fragment nuclides; washing and eluting acids are respectively dissolved in water to form an aqueous washing liquid and an aqueous eluting liquid; the washing and eluting acids are one of nitric acid and hydrochloric acid, or a mixture of diethylenetriaminepentaacetic acid and lactic acid, and the concentration of the washing and eluting acids is 0.01 to 10 mol / L; RE or TRU resin, P 204 Or HDEHP resin, BCPDTPA resin, and DN resin are respectively loaded into chromatography adsorption columns.

[0089] Among them, RE or TRU chromatography adsorption column is mainly used to separate Am, Cm, Ce, Nd, Sm, Eu, Tb from other actinides and fission products; 204 Or HDEHP chromatography adsorption column is mainly used to achieve further separation of Am, Cm, Ce, Nd, Sm, Eu, Tb from other actinides and fission products, separation of Am, Cm from Ce, Nd, Sm, Eu, Tb, and separation of Ce, Tb from Nd, Sm, Eu; BCPDTPA chromatography adsorption column is mainly used to achieve separation of Am from Cm; DN chromatography adsorption column is mainly used to achieve separation of Nd, Sm, Eu from each other and from other fission products.

[0090] Step 2: using a peristaltic pump for delivery and a solenoid valve for gating, the radioactive sample containing trivalent actinide elements and rare earth fragment nuclides is separated and adsorbed through the RE or TRU chromatography adsorption column 16, and the effluent is collected as waste liquid;

[0091] Step 3: Use a peristaltic pump to deliver and a solenoid valve to select so that the washing liquid passes through the RE or TRU chromatography adsorption column 16 for washing, and the effluent is collected as waste liquid;

[0092] Step 4: Use the peristaltic pump to deliver and the solenoid valve to select, so that the first column eluent passes through the RE or TRU chromatography adsorption column 16 and P in turn. 204 or HDEHP chromatography column 17 for desorption and re-adsorption of trivalent actinide elements and rare earth fragment nuclides, and the effluent is collected as waste liquid;

[0093] Step 5: 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 P 204 Or the HDEHP chromatography adsorption column 17 is washed, and the effluent is collected as waste liquid;

[0094] Step 6: Use the peristaltic pump to deliver and the solenoid valve to select, so that the second-stage eluent of the second-stage column passes through P 204 or HDEHP chromatography adsorption column 17 for desorption of trivalent actinide, and the effluent is collected in the first-stage eluent reservoir 10 of the third-stage column;

[0095] Step 7: Use the peristaltic pump to deliver and the solenoid valve to select, so that the second column and the third stage eluent pass through P 204 Or the HDEHP chromatography adsorption column 17 is washed, and the effluent is collected as waste liquid;

[0096] Step 8: Use the peristaltic pump to deliver and the solenoid valve to select, so that the second column and the fourth stage eluent pass through P in sequence. 204 or 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 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 γ-radioactive solution of terbium, 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: 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; the effluent, i.e., the radioactive solution of curium, 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: Use a peristaltic pump to deliver and a solenoid valve to select so that the third-stage eluent of the third-stage column passes through the BCPDTPA chromatography adsorption column 18; 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: 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; the effluent, i.e., the γ-radioactive solution of neodymium, is collected in the neodymium product collector 26;

[0106] Step 18: 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; 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 an electromagnetic 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 solution of europium, 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 10 mL 2 mol / L HNO 3 , add sodium nitrite, heat to 90-100 degrees, cool to form a solution containing trivalent actinide elements and rare earth fragment nuclides, place the solution in a storage tank 1, and its γ radioactivity 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 25mL 2mol / L HNO in the washing solution reservoir 2 3 The solution is washed at a flow rate of 1.5 mL / min through a RE or TRU chromatography column 16 to achieve further separation of Mo and Tc, Te, I, Ba, Ru, Rh, Nb, etc. The effluent is collected in a waste liquid collector 27.

[0114] Use 25mL 0.05mol / L HNO in the first column eluent reservoir 3 3 The solution was controlled at a flow rate of 1.0 mL / min and passed through 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 a HDEHP chromatography adsorption column to achieve desorption and re-adsorption of trivalent actinide elements and rare earth fragment nuclides, and the effluent is collected in a waste liquid collector 27.

[0115] Use 25mL 0.1mol / L HNO in the first eluent reservoir 4 of the second column 3 solution, controlling the flow rate at 1.0 mL / min, through P 204 Or the HDEHP chromatography adsorption column 17 is washed, and the effluent is collected in the 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 eluent reservoir 5 of the second-stage column at a flow rate of 1.0 mL / min through P 204 Or HDEHP chromatography adsorption column 17 for elution, and the effluent is collected in the third column first stage eluent reservoir 10; wherein the third column first stage eluent reservoir 10 is pre-filled with 1.2mL 10mol / LHNO 3 Solution.

[0117] Use 40mL 0.2mol / L HNO in the third eluent reservoir 6 of the second column3 -0.07mol / LNaBrO 3 solution, controlling the flow rate at 1.0 mL / min, through P 204 Or the HDEHP chromatography adsorption column 17 is used for elution, and the effluent is collected in the waste liquid collector 27.

[0118] Use 20mL 1mol / L HNO in the fourth eluent reservoir 7 of the second column 3 -0.07mol / LNaBrO 3 solution, controlling the flow rate at 1.0 mL / min, and passing through P 204 Or the HDEHP chromatographic adsorption column 17 and the DN chromatographic adsorption column 19 are eluted, wherein the DN chromatographic adsorption column 19 is A DN chromatography adsorption column is used to achieve desorption and re-adsorption of samarium, europium and neodymium, and the effluent is collected in a waste liquid collector 27.

[0119] Use 20mL 0.1mol / L HNO in the first eluent reservoir 4 of the second column 3 Solution, control the flow rate to 1.0mL / min, and pass through P again 204 Or the HDEHP chromatography adsorption column 17 is washed, and the effluent is collected in the waste liquid collector 27.

[0120] Use 15mL 1mol / L HNO in the fifth eluent reservoir 8 of the second column 3 solution, controlling the flow rate at 1.0 mL / min, through P 204 Or HDEHP chromatography adsorption column 17, the effluent is collected in the cerium product collector 22, which is the gamma radioactive measurement source of cerium.

[0121] Use 15mL 3mol / L HNO in the sixth eluent reservoir 9 of the second column 3 solution, controlling the flow rate to 0.5 mL / min, through P 204 Or HDEHP chromatography adsorption column 17, the effluent is collected in the terbium product collector 23, which is the gamma 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 is 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 15mL 0.1mol / L HNO in the second eluent reservoir 11 of the third column 3The solution is passed through the BCPDTPA chromatography adsorption column 18 at a controlled flow rate of 1.0 mL / min; the effluent, i.e., the γ-radioactive solution of curium, is collected in the curium product collector 20.

[0124] Use 15mL 0.1mol / L HNO in the second eluent reservoir 11 of the third column 3 The solution is eluted again through the BCPDTPA chromatography adsorption column 18 at a controlled flow rate of 1.0 mL / min, and the effluent is collected in the waste liquid collector 27.

[0125] Use 8 mL 1 mol / L HNO in the third eluent reservoir 12 of the third column 3 The solution is passed through the BCPDTPA chromatography adsorption column 18 at a controlled flow rate of 1.0 mL / min; 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 through the DN chromatography adsorption column 19 at the same time, and collect the effluent 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 gamma radioactive measurement source of neodymium.

[0128] Use 10mL of 1.5mol / L HCl solution in the second eluent reservoir 14 of the fourth column, control the flow rate to 0.5mL / min, pass through the DN chromatography adsorption column 19, and collect the effluent in the samarium product collector 24, which is the γ-radioactivity measurement source 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 10mL 0.1mol / L HCl solution in the third-stage eluent reservoir 15 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 europium product collector 25, which is the gamma radioactive measurement source of europium.

[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 7The 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 is replaced by 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, terbium, etc. The recovery rates 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 actinide elements and rare earth fragment nuclides, characterized in that: It comprises 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 chromatographic separation unit through the delivery pump (30), and the liquid flowing out of the chromatographic 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 via pipelines, 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); 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) which are 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 also comprises a microcomputer, and the microcomputer is used for controlling the solenoid 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 chromatographic separation unit, the waste liquid collector (27), and the product collection unit is as follows: A radioactive solution storage tank (1) containing trivalent actinide elements and rare earth fragment nuclides, 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 eluent storage tank (11) of the third column, the third eluent storage tank (12) of the third column, the first eluent storage tank (13) of the fourth column, the second eluent storage tank (14) of the fourth column, and the third eluent storage tank (15) of the fourth column are connected to the corresponding inlet 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), P 204 or the feed inlet of the HDEHP chromatographic adsorption column (17), the BCPDTPA chromatographic adsorption column (18), or the DN chromatographic adsorption column (19); the discharge port of the RE or TRU chromatographic adsorption column (16) is connected to the P through a valve (31). 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 actinide elements and rare earth fragment nuclides, using any separation device according to claims 1 to 4, characterized in that: The steps include: Step 1, preparation before separation: The radioactive sample containing trivalent actinide elements and rare earth fragment nuclides to be separated is dissolved in nitric acid, sodium nitrite is added, and the mixture is heated and cooled at a temperature of 90 to 100° C. to obtain an aqueous radioactive sample containing trivalent actinide elements and rare earth fragment nuclides; The washing and eluting acids are dissolved in water respectively to obtain an aqueous washing liquid and an aqueous eluting liquid; the washing and eluting acids are one of nitric acid and 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 the 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 fragment nuclides: The aqueous radioactive sample containing trivalent actinides and rare earth fragment nuclides prepared in step 1 is placed in a radioactive solution storage tank containing trivalent actinides and rare earth fragment nuclides (1), and the aqueous radioactive sample containing actinides and lanthanide fission products is separated and adsorbed using an RE or TRU chromatographic adsorption column (16), 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 liquid, washing the RE or TRU chromatography adsorption column (16), and collecting the effluent into a waste liquid collector (27); Step 4, rinse: Use aqueous eluent to wash the RE or TRU chromatography column (16), P 204 Or a HDEHP chromatography adsorption column (17), a DN chromatography adsorption column (19), and a BCPDTPA chromatography adsorption column (18) 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.

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 actinide elements and rare earth fragment nuclides 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 first-stage column eluent, the second-stage column first-stage eluent, the second-stage column second-stage eluent, the second-stage column third-stage eluent, the second-stage column fourth-stage eluent, the second-stage column fifth-stage eluent, the second-stage column sixth-stage eluent, the third-stage column first-stage eluent, the third-stage column second-stage eluent, the third-stage column third-stage eluent, the fourth-stage column first-stage eluent, the fourth-stage column second-stage eluent, and the fourth-stage column third-stage eluent, 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, and the flow rate is 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, and the flow rate was 1.0 mL / min; The third eluent of the second column is 0.2mol / L HNO3-0.07mol / LNaBrO3 solution, and the flow rate is 1.0mL / min; the fourth eluent of the second column is 1mol / L HNO3-0.07mol / LNaBrO3 solution, and the flow rate is 1.0mL / min; the fifth eluent of the second column is 1mol / L HNO3 solution, and the flow rate is 1.0mL / min; The sixth stage eluent of the second stage column is 3 mol / L HNO3 solution, and the flow rate is 0.5 mL / min; The first eluent of the third column was 0.05mol / LDTPA-1mol / L lactic acid solution at a flow rate of 1.0mL / min; the second eluent of the third column was 0.1mol / LHNO3 solution at a flow rate of 1.0mL / min; The third-stage eluent of the third-stage column is 1 mol / L HNO3 solution, and the flow rate is 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, elution, further comprises: The first column eluent passes through the RE or TRU chromatography adsorption column (16) and P 204 or a HDEHP chromatography column (17) for desorption and re-adsorption of trivalent actinide elements 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 a waste liquid collector (27); The second column second stage eluent passes through P 204 or a HDEHP chromatography adsorption column (17) to desorb trivalent actinides, and the effluent is collected in a first-stage eluent storage tank (10) of a third-stage column; The second column and the third eluent pass through P 204 or HDEHP chromatography adsorption column (17), washing, and collecting the effluent into a waste liquid collector (27); The second column and the fourth eluent pass through P 204 or a HDEHP chromatography adsorption column (17) and a DN chromatography adsorption column (19) to desorb and re-adsorb samarium, europium and neodymium, and the effluent is collected in 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 a waste liquid collector (27); The fifth stage eluent of the second column passes through P 204 or a HDEHP chromatography column (17), the effluent is collected in a cerium product collector (22) to obtain a γ-radioactive solution of cerium; The sixth stage eluent of the second column passes through P 204 or a HDEHP chromatography adsorption column (17), the effluent is collected in 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 a DN chromatography adsorption column (19), and the effluent is collected in a neodymium product collector (26) to obtain a neodymium gamma-radioactive solution; The second-stage eluent of the fourth-stage column passes through a DN chromatography adsorption column (19), and the effluent is collected in a samarium product collector (24) to obtain a samarium gamma-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: The trivalent actinide elements are isotopes of americium and curium, and the rare earth fragment nuclides are isotopes of cerium, neodymium, samarium, europium, and terbium.

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