Separation device and separation method for actinide and lanthanide fission products

Abstract

The invention relates to a separation device and a separation method for actinide and lanthanide fission products, belongs to the technical field of separation of actinide 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 steps of preparation before separation, adsorption of actinide and lanthanide fission products, washing and leaching. The method is used for separating actinide and lanthanide fission products.

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 actinide elements and lanthanide fission products. Background Art

[0002] In order to achieve sustainable development of nuclear energy, uranium-plutonium mixed fuel prepared from actinide elements uranium and plutonium has become a new type of nuclear fuel (MOX fuel). The mixed fuel includes a variety of U isotopes (such as U-234, U-235, U-238, etc.) and a variety of Pu isotopes (such as Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, etc.), among which Pu-241 (half-life 14.29 years) is converted into Am-241 (half-life 432.2 years) through radioactive decay. Uranium-plutonium fissionable nuclides undergo fission reactions under the action of neutrons, producing hundreds of radioactive fission products. Carrying out radiochemical analysis of actinide elements and fission products is of great significance to many research and application fields such as reactor burnup monitoring, nuclear decay data measurement, fission yield measurement, nuclear waste treatment, and nuclear forensics.

[0003] The content of actinide elements such as uranium, plutonium, and americium in samples is usually at a trace or trace level. The radiochemical analysis is mainly carried out by measuring the content of their main isotopes U-238, Pu-239, and Am-241 through mass spectrometers or α spectrometers. However, there is mutual interference in the measurement of these isotopes. For example, the mass spectrometry measurement of Pu-239 will be interfered by the hydrogen ion complex of uranium-238; U-238 and Pu-238 are isotopic interferences with each other in mass spectrometry; Am-241 and Pu-241 are isotopic interferences with each other in mass spectrometry, and Am-241 (5.485MeV) will be interfered by the heavy peak of Pu-238 in α spectrum measurement. Therefore, the separation and purification of plutonium, uranium, and americium and the elimination of mutual interference are crucial for the accurate quantitative analysis of their isotopes.

[0004] Among the large number of fission products generated by neutron-induced uranium-plutonium nuclear materials, lanthanide gamma-radioactive fission products such as cerium, neodymium, samarium, europium, and terbium are the focus of analysis. Among them, cerium fission products Ce-141 (half-life 32.4 days) and Ce-144 (half-life 284 days), neodymium fission products Nd-147 (half-life 11.1 days), they have medium-life half-lives and high fission yields. Samarium fission products Sm-153 (half-life 46.8 hours), europium fission products Eu-155 (half-life 4.96 years) and Eu-156 (15.2 days), terbium fission products Tb-161 (half-life 6.91 days), their fission yields are relatively low and difficult to detect. Although these lanthanide fission products have different fission yields and half-lives, their γ-radioactivity in the sample is relatively low, and a trap-type high-purity germanium detection spectrometer is usually used to measure and analyze their activity. Since the uranium-plutonium fission process also produces a large number of other types of fission products that are very rich in γ rays, such as Mo-99, Tc-99m, Te-132, Ru-103, I-131, I-132, Ba-140, La-140, Zr-95, Nb-95, etc., the Compton plateau and spectrum peak interference are very serious, and there is also spectrum peak interference between lanthanide fission products. Therefore, it is necessary to solve the problem of decontamination of lanthanide fission products with each other and other interfering nuclides through radiochemical separation, so as to obtain the corresponding measurement source of radiochemical purity to achieve accurate measurement and analysis of activity.

[0005] 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 separation of gamma-radioactive lanthanide fission products and other interfering nuclides.

[0006] Modolo et al., Recovery of actinides and lanthanides from high-level liquid waste by extraction chromatography using TODGA+TBP impregnated resins. Radiochim. Acta., 2007, 95: 391-397, reported a method of using TODGA+TBP resin to recover actinides (uranium, thorium, americium, curium, californium) and lanthanides (cerium, neodymium, samarium, europium, gadolinium, etc.) from high-level liquid waste, and achieved separation from other fission products (Mo, Ru, Zr, etc.). However, this method has not effectively solved the problem of separation between actinides and lanthanides and their groups, and is only suitable for the co-enrichment or recovery of actinides and lanthanides.

[0007] 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 separation method cannot meet the technical requirements for high-precision test and analysis of actinide and lanthanide fission products in the fields of basic nuclear data measurement and nuclear energy development. Summary of the invention

[0008] In order to overcome the shortcomings of low decontamination and low recovery rate in the separation of actinide and lanthanide fission products, the present invention provides a separation device and a separation method for actinide and lanthanide fission products.

[0009] The technical solution adopted by the present invention to solve the technical problem is:

[0010] A device for separating actinide and lanthanide fission products comprises a liquid storage tank unit, a chromatographic separation unit, a waste liquid collector, a product collection unit and a delivery pump.

[0011] 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;

[0012] 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.

[0013] 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;

[0014] The storage tank unit includes a radioactive solution storage tank containing actinide and lanthanide fission products, a washing liquid storage tank, a first-stage column first-stage eluent storage tank, a first-stage column second-stage eluent storage tank, a first-stage column third-stage eluent storage tank, a first-stage column fourth-stage 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 second-stage column seventh-stage eluent storage tank, a third-stage column first-stage eluent storage tank, a third-stage column second-stage eluent storage tank, and a third-stage column third-stage eluent storage tank.

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

[0016] The chromatographic separation unit includes a TRU or RE chromatographic adsorption column, a HDEHP or P 204 Chromatography adsorption column, DN chromatography adsorption column.

[0017] 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.

[0018] The above separation device also includes a microcomputer, which is used to control the solenoid valve and the peristaltic pump.

[0019] 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:

[0020] The outlets of the radioactive solution reservoir containing actinide and lanthanide fission products, the washing solution reservoir, the first-stage column first-stage eluent reservoir, the first-stage column second-stage eluent reservoir, the first-stage column third-stage eluent reservoir, the first-stage column fourth-stage eluent reservoir, the second-stage column first-stage eluent reservoir, the second-stage column second-stage eluent reservoir, the second-stage column third-stage eluent reservoir, the second-stage column fourth-stage eluent reservoir, the second-stage column fifth-stage eluent reservoir, the second-stage column sixth-stage eluent reservoir, the second-stage column seventh-stage eluent reservoir, the third-stage column first-stage eluent reservoir, the third-stage column second-stage eluent reservoir, and the third-stage eluent reservoir of the third column are connected to the corresponding inlet of the delivery pump through valves; the outlet of the delivery pump is respectively connected to the TRU or RE chromatographic adsorption column, HDEHP or P through valves. 204 The inlet of the chromatographic adsorption column and the DN chromatographic adsorption column are connected; the outlet of the TRU or RE chromatographic adsorption column is connected to the uranium product collector, the plutonium product collector, the HDEHP or P through a valve. 204 The inlet of the chromatography adsorption column is connected to the waste liquid collector; HDEHP or P 204 The discharge port of the chromatography adsorption column is connected to the americium product collector, the terbium product collector, the europium product collector, the samarium product collector, the DN chromatography adsorption column inlet and the waste liquid collector through valves; the discharge port of the DN chromatography adsorption column is connected to the neodymium product collector, the cerium product collector and the waste liquid collector through valves.

[0021] A method for separating actinide and lanthanide fission products comprises the following steps:

[0022] Step 1, Preparation before Isolation

[0023] The radioactive sample containing actinide elements and lanthanide fission products to be separated is dissolved in nitric acid, sodium nitrite is added, and the mixture is heated and cooled at 90-100° C. to obtain an aqueous radioactive sample containing actinide elements and lanthanide fission products.

[0024] The washing and rinsing acids are dissolved in water respectively to obtain aqueous washing liquid and aqueous rinsing liquid; the washing and rinsing acids are one of nitric acid and hydrochloric acid, or a mixture of two of nitric acid, hydrochloric acid, hydrofluoric acid, diethylenetriaminepentaacetic acid, lactic acid and ascorbic acid.

[0025] TRU or RE resin, HDEHP or P 204 Resin and DN resin are respectively loaded into chromatographic adsorption columns to obtain TRU or RE chromatographic adsorption columns, HDEHP or P 204 Chromatography adsorption column, DN chromatography adsorption column.

[0026] Step 2, Adsorption of actinide and lanthanide fission products

[0027] The aqueous radioactive sample containing actinide and lanthanide fission products prepared in step 1 is placed in a storage tank for radioactive solution containing actinide and lanthanide fission products, and a TRU or RE chromatographic adsorption column is used to separate and adsorb the aqueous radioactive sample containing actinide and lanthanide fission products. The actinide and lanthanide fission products are adsorbed in the TRU or RE chromatographic adsorption column, and the effluent is collected in a waste liquid collector.

[0028] Step 3, Washing

[0029] Use aqueous washing liquid to wash the TRU or RE chromatography adsorption column, and collect the effluent into the waste liquid collector;

[0030] Step 4, rinse

[0031] Use aqueous eluent to adsorb TRU or RE chromatography columns, HDEHP or P 204 The chromatography adsorption column and the DN chromatography adsorption column are eluted to obtain a gamma radioactive solution of europium, a gamma radioactive solution of terbium, a gamma radioactive solution of cerium, and a gamma radioactive solution of neodymium.

[0032] In the above separation method, in the preparation before separation of step 1, the concentration of nitric acid used to dissolve the radioactive sample containing actinide elements and lanthanide fission products to be separated is 1 mol / L to 4 mol / L, and the concentration of acid used for washing and eluting is 0.01 to 6.0 mol / L. In the above separation method, in the preparation before separation of 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.

[0033] In the above separation method, in the preparation before separation in step 1, the aqueous eluent includes the first eluent of the first column, the second eluent of the first column, the third eluent of the first column, the fourth 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 seventh eluent of the second column, the first eluent of the third column, the second eluent of the third column, the second eluent of the third column, and the third eluent of the third column. The aqueous eluent is placed in the corresponding eluent reservoir of the reservoir unit.

[0034] The first eluent of the first column is 0.01mol / L~0.1mol / L HNO3 solution, the second eluent of the first column is 0.01mol / L~0.5mol / L HNO3 solution containing 0.01mol / L~0.1mol / L ACB, the third eluent of the first column is 0.5mol / L~2mol / L HCl solution containing 0.01mol / L~0.03mol / L HF, the fourth eluent of the first column is 0.05mol / L~0.2mol / L HCl solution containing 0.1mol / L~0.4mol / L HF. HCl solution, the first eluent of the second column is 0.01mol / L~0.1mol / LHNO3 solution, the second eluent of the second column is 0.5mol / L~1.5mol / L lactic acid solution containing 0.04mol / L~0.08mol / L DTPA, the third eluent of the second column is 0.15mol / L~0.25mol / LHNO3 solution, the fourth eluent of the second column is 0.25mol / L-0.45mol / L HNO3 solution, the fifth eluent of the second column is 0.5mol / L~0.75mol / L HNO3 solution, the sixth eluent of the second column is 0.8mol / L~2mol / L HNO3 solution, the seventh eluent of the second column is 2.5mol / L~4mol / L HNO3 solution, the first eluent of the third column is 0.3mol / L~0.5mol / L HNO3 solution, the second-stage eluent of the third-stage column is 2mol / L~3mol / L HCl solution, and the third-stage eluent of the third-stage column is 0.1mol / L~1.5mol / L HCl solution.

[0035] In the above separation method, the step 4, elution, further comprises:

[0036] First column The first eluent passes through the TRU or RE chromatography adsorption column and HDEHP or P 204 The chromatographic adsorption column desorbs and re-adsorbs the americium and lanthanide fission products, and the effluent is collected in a waste liquid collector;

[0037] The second stage eluent of the first stage column passes through a TRU or RE chromatographic adsorption column, and the effluent is collected in a plutonium product collector to obtain a radioactive plutonium solution.

[0038] The third-stage eluent of the first-stage column passes through a TRU or RE chromatographic adsorption column, and the effluent is collected in a plutonium product collector to obtain a radioactive plutonium solution.

[0039] The fourth-stage eluent of the first-stage column passes through a TRU or RE chromatographic adsorption column, and the effluent is collected in a uranium product collector to obtain a radioactive uranium solution.

[0040] The first eluent of the second column is HDEHP or P 204 The chromatographic adsorption column is washed and the effluent flows to the waste liquid collector.

[0041] The second column second stage eluent is HDEHP or P 204 Chromatographic adsorption column; the effluent is collected in an americium product collector to obtain a radioactive solution of americium.

[0042] The second column and the third eluent are HDEHP or P 204 The chromatographic adsorption column is washed and the effluent is collected in a waste liquid collector.

[0043] The fourth stage eluent of the second column is successively passed through HDEHP or P 204 The chromatographic adsorption column and the DN chromatographic adsorption column are used to desorb and re-adsorb cerium and neodymium, and the effluent is collected in a waste liquid collector.

[0044] The fourth stage eluent of the second column is HDEHP or P 204 The chromatographic adsorption column is washed and the effluent is collected in a waste liquid collector.

[0045] The fifth stage eluent of the second column is HDEHP or P 204 The effluent is collected into a samarium product collector through a chromatography adsorption column to obtain a samarium γ-radioactive solution.

[0046] The fifth stage eluent of the second column is HDEHP or P 204 The chromatographic adsorption column is washed and the effluent flows to the waste liquid collector.

[0047] The sixth stage eluent of the second stage column is HDEHP or P 204 The effluent is collected into a europium product collector to obtain a europium γ-radioactive solution.

[0048] The seventh stage eluent of the second column is HDEHP or P 204 The effluent is collected into a terbium product collector to obtain a terbium gamma radioactive solution.

[0049] The first-stage eluent of the third-stage column is washed through the DN chromatography adsorption column, and the effluent is collected in the waste liquid collector.

[0050] The second-stage eluent of the third-stage column is passed through the DN chromatographic adsorption column, and the effluent is collected in a cerium product collector to obtain a γ-radioactive solution of cerium.

[0051] The second-stage eluent of the third-stage column is washed through the DN chromatography adsorption column, and the effluent is collected in the waste liquid collector.

[0052] The third-stage column: The third-stage eluent passes through the DN chromatographic adsorption column, and the effluent is collected in the neodymium product collector to obtain a neodymium γ-radioactive solution.

[0053] In the above separation method, the actinide elements are isotopes including uranium, plutonium and americium, and the lanthanide fission products are isotopes including cerium, neodymium, samarium, europium and terbium.

[0054] The beneficial effects of the present invention are:

[0055] A method for separating actinide and lanthanide fission products, which effectively utilizes the difference in chemical complexing behavior between actinide elements uranium, plutonium, americium and lanthanide fission products cerium, neodymium, samarium, europium and terbium on different chromatographic adsorption columns, so that uranium and plutonium are adsorbed on TRU or RE chromatographic adsorption columns, and americium, samarium, europium and terbium are adsorbed on HDEHP or P 204 Chromatographic adsorption column, cerium and neodymium are adsorbed on the DN chromatographic adsorption column, and through elution and desorption, the integrated high-selective separation and recovery of actinide and lanthanide elements such as uranium, plutonium, americium, cerium, neodymium, samarium, europium and terbium are achieved.

[0056] A separation method for actinide and lanthanide fission products, with clear separation unit functions, ingenious connection of column media, and easy flow rate control. A streamlined automatic control separation process of simultaneous adsorption, elution, and desorption is constructed using a simple three-stage separation unit.

[0057] A method for separating actinide elements and lanthanide fission products. The entire separation process from the absorption of original radioactive liquid to the preparation of actinide elements uranium, plutonium and americium and lanthanide fission products 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.

[0058] A method for separating actinide elements and lanthanide fission products, compared with the existing method, realizes the synchronous and efficient separation of actinide elements uranium, plutonium, americium and lanthanide fission products cerium, neodymium, samarium, europium and terbium under automatic control conditions; the recovery rate of uranium, plutonium, americium, cerium, neodymium, samarium, europium and terbium is 85% to 97%, and the decontamination factor between actinides is within 10 3 ~10 5 The decontamination factor between lanthanide fission products is 10 2 ~10 5 The decontamination factor for other fission products is 10 4 ~10 6 . BRIEF DESCRIPTION OF THE DRAWINGS

[0059] Figure 1 This is a schematic diagram of a separation device according to Example 1 of the present invention;

[0060] Figure 2 The γ-radiation energy spectrum of the original solution containing actinide elements and lanthanide fission products used in Example 1 of the present invention;

[0061] Figure 3 The radioactivity spectrum of samarium gamma, a lanthanide fission product separated and obtained in Example 1 of the present invention;

[0062] Figure 4 This is the radioactivity spectrum of europium gamma, a lanthanide fission product separated and obtained in Example 1 of the present invention;

[0063] Figure 5 This is the terbium gamma radioactivity spectrum of the lanthanide fission product separated in Example 1 of the present invention;

[0064] Figure 6 This is the radioactivity spectrum of cerium gamma, a lanthanide fission product separated in Example 1 of the present invention;

[0065] Figure 7 This is the radioactivity spectrum of neodymium gamma, a lanthanide fission product separated in Example 1 of the present invention.

[0066] The reference numerals are as follows:

[0067] 1. A reservoir for radioactive solution containing actinide and lanthanide fission products, 2. A reservoir for washing solution, 3. A reservoir for first-stage eluent of the first column, 4. A reservoir for second-stage eluent of the first column, 5. A reservoir for third-stage eluent of the first column, 6. A reservoir for fourth-stage eluent of the first column, 7. A reservoir for first-stage eluent of the second column, 8. A reservoir for second-stage eluent of the second column, 9. A reservoir for third-stage eluent of the second column, 10. Second column fourth eluent reservoir, 11. Second column fifth eluent reservoir, 12. Second column sixth eluent reservoir, 13. Second column seventh eluent reservoir, 14. Third column first eluent reservoir, 15. Third column second eluent reservoir, 16. Third column third eluent reservoir, 17. TRU or RE chromatography adsorption column, 18. HDEHP or P 204 Chromatographic adsorption column, 19. DN chromatographic adsorption column, 20. Uranium product collector, 21. Plutonium product collector, 22. Americium product collector, 23. Terbium product collector, 24. Europium product collector, 25. Samarium product collector, 26. Neodymium product collector, 27. Cerium product collector, 28. Waste liquid collector, 30. Transfer pump, 31. Valve. DETAILED DESCRIPTION

[0068] The present invention is further described in detail below with reference to the accompanying drawings and specific embodiments.

[0069] like Figure 1As shown, the separation device of the radioactive solution containing actinide elements and lanthanide fission products of the present invention comprises a liquid storage tank unit, a chromatographic separation unit, a waste liquid collector 28, 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 nuclide radiation on the human body during separation, and reduce the labor intensity of personnel. The peristaltic pump uses a hose extrusion method to deliver the separation liquid, and the flow rate and flow velocity of the liquid are controlled by the rotation speed of the peristaltic pump.

[0070] The above-mentioned storage tank unit includes a radioactive solution storage tank 1 containing actinide and lanthanide fission products, a washing liquid storage tank 2, a first-stage column first-stage eluent storage tank 3, a first-stage column second-stage eluent storage tank 4, a first-stage column third-stage eluent storage tank 5, a first-stage column fourth-stage eluent storage tank 6, a second-stage column first-stage eluent storage tank 7, a second-stage column second-stage eluent storage tank 8, a second-stage column third-stage eluent storage tank 9, a second-stage column fourth-stage eluent storage tank 10, a second-stage column fifth-stage eluent storage tank 11, a second-stage column sixth-stage eluent storage tank 12, a second-stage column seventh-stage eluent storage tank 13, a third-stage column first-stage eluent storage tank 14, a third-stage column second-stage eluent storage tank 15, and a third-stage column third-stage eluent storage tank 16. Each storage tank is connected to a corresponding chromatographic adsorption column through a valve and a pump to achieve different functions.

[0071] The above-mentioned chromatography separation unit includes a TRU or RE chromatography adsorption column 17, HDEHP or P 204 Chromatography adsorption column 18, DN chromatogram adsorption column 19.

[0072] The product collecting unit includes a uranium product collector 20 , a plutonium product collector 21 , an americium product collector 22 , a terbium product collector 23 , a europium product collector 24 , a samarium product collector 25 , a neodymium product collector 26 , and a cerium product collector 27 .

[0073] The connection relationship between the above-mentioned storage tanks and the chromatographic adsorption column is as follows: a storage tank 1 for a radioactive solution containing actinide elements and lanthanide fission products, a storage tank 2 for a washing solution, a storage tank 3 for a first-stage column first-stage eluent, a storage tank 4 for a first-stage column second-stage eluent, a storage tank 5 for a first-stage column third-stage eluent, a storage tank 6 for a first-stage column fourth-stage eluent, a storage tank 7 for a second-stage column first-stage eluent, a storage tank 8 for a second-stage column second-stage eluent, a storage tank 9 for a second-stage column third-stage eluent, and a storage tank 4 for a second-stage column fourth-stage eluent 10, the fifth eluent reservoir 11 of the second column, the sixth eluent reservoir 12 of the second column, the seventh eluent reservoir 13 of the second column, the first eluent reservoir 14 of the third column, the second eluent reservoir 15 of the third column, and the third eluent reservoir 16 of the third 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 TRU or RE chromatographic adsorption column 17, HDEHP or P through a valve. 204 The discharge port of the TRU or RE chromatography adsorption column 17 is connected to the uranium product collector 20, the plutonium product collector 21, the HDEHP or P through the valve 31. 204 The feed port of the chromatographic adsorption column 18 is connected to the waste liquid collector 28; HDEHP or P 204 The discharge port of the chromatography adsorption column 18 is connected to the americium product collector 22, the terbium product collector 23, the europium product collector 24, the samarium product collector 25, the feed port of the DN chromatography adsorption column 19 and the waste liquid collector 28 through a valve 31; the discharge port of the DN chromatography adsorption column 19 is connected to the neodymium product collector 26, the cerium product collector 27 and the waste liquid collector 28 through a valve 31.

[0074] The separation step of the present invention is:

[0075] Step 1: Preparation before separation

[0076] The radioactive sample containing actinide elements and lanthanide fission products 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 solution; 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 two of nitric acid, hydrochloric acid, hydrofluoric acid, diethylenetriaminepentaacetic acid, lactic acid, and ascorbic acid, and the concentration of the washing and eluting acids is 0.01 to 6.0 mol / L; TRU or RE resin, HDEHP or P 204 Resin and DN resin are respectively loaded into chromatography adsorption columns.

[0077] Among them, TRU or RE chromatography adsorption column is mainly used to separate U, Pu, Am, Ce, Nd, Sm, Eu, Tb from other fission products, and to separate U, Pu from Am, Ce, Nd, Sm, Eu, Tb; HDEHP or P 204 The chromatographic adsorption column is mainly used to further separate Am, Ce, Nd, Sm, Eu, Tb from other fission products, to separate Am from Ce, Nd, Sm, Eu, Tb, and to separate Ce, Nd from Sm, Eu, Tb; the DN chromatographic adsorption column is mainly used to separate Ce from Nd.

[0078] Step 2: using a peristaltic pump for delivery and a solenoid valve for gating, the radioactive sample containing actinide elements and lanthanide fission products is separated and adsorbed through a TRU or RE chromatography adsorption column 17, and the effluent is collected as waste liquid;

[0079] Step 3: Use a peristaltic pump to deliver and a solenoid valve to select, so that the washing liquid passes through the TRU or RE chromatography adsorption column 17 for washing, adsorption and separation, and the effluent is collected as waste liquid;

[0080] Step 4: Use the peristaltic pump to deliver and the solenoid valve to select, so that the first-stage eluent of the first-stage column passes through the TRU or RE chromatography adsorption column 17 and HDEHP or P in sequence. 204 The chromatographic adsorption column 18 performs desorption and re-adsorption of americium and lanthanide fission products, and the effluent is collected as waste liquid;

[0081] Step 5: Use a peristaltic pump to deliver and a solenoid valve to select so that the first-stage column and the second-stage eluent pass through the TRU or RE chromatography adsorption column 17; the effluent, i.e., the radioactive solution of plutonium, is collected in the plutonium product collector 21;

[0082] Step 6: Use a peristaltic pump to deliver and a solenoid valve to select so that the third-stage eluent of the first-stage column passes through the TRU or RE chromatography adsorption column 17; the effluent, i.e., the radioactive solution of plutonium, is collected in the plutonium product collector 21;

[0083] Step 7: Use a peristaltic pump to deliver and a solenoid valve to select so that the fourth-stage eluent of the first-stage column passes through the TRU or RE chromatography adsorption column 17; the effluent, i.e., the radioactive solution of uranium, is collected in the uranium product collector 20;

[0084] Step 8: Use the peristaltic pump to deliver and the solenoid valve to select, and make the first stage eluent of the second stage column pass through HDEHP or P 204 The chromatographic adsorption column 18 is washed, and the effluent is collected as waste liquid;

[0085] Step 9: 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 HDEHP or P 204Chromatographic adsorption column 18; the effluent, i.e., the radioactive solution of americium, is collected in the americium product collector 22;

[0086] Step 10: Use the peristaltic pump to deliver and the solenoid valve to select, so that the second column and the third stage eluent pass through HDEHP or P 204 The chromatographic adsorption column 18 is washed, and the effluent is collected as waste liquid;

[0087] Step 11: Use the peristaltic pump to deliver and the solenoid valve to select, so that the fourth stage eluent of the second stage column passes through HDEHP or P in turn. 204 The chromatographic adsorption column 18 and the DN chromatographic adsorption column 19 perform desorption and re-adsorption of cerium and neodymium, and the effluent is collected as waste liquid;

[0088] Step 12: Use the peristaltic pump to deliver and the solenoid valve to select, so that the fourth stage eluent of the second stage column passes through HDEHP or P 204 The chromatographic adsorption column 18 is washed, and the effluent is collected as waste liquid;

[0089] Step 13: 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 HDEHP or P 204 Chromatographic adsorption column 18; the effluent, i.e., the γ-radioactive solution of samarium, is collected in the samarium product collector 25;

[0090] Step 14: 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 HDEHP or P 204 The chromatographic adsorption column 18 is washed, and the effluent is collected as waste liquid;

[0091] Step 15: 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 HDEHP or P 204 Chromatographic adsorption column 18; the effluent, i.e., the γ-radioactive solution of europium, is collected in the europium product collector 24;

[0092] Step 16: Use the peristaltic pump to deliver and the solenoid valve to select, so that the seventh stage eluent of the second stage column passes through HDEHP or P 204 Chromatographic adsorption column 18; the effluent, i.e., the γ-radioactive solution of terbium, is collected in the terbium product collector 23;

[0093] Step 17: 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 DN chromatography adsorption column 19 for washing, and the effluent is collected as waste liquid;

[0094] Step 18: 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 DN chromatography adsorption column 19; the effluent, i.e., the γ-radioactive solution of cerium, is collected in the cerium product collector 27;

[0095] Step 19: Use a peristaltic pump to deliver and a solenoid valve to select so that the second-stage eluent of the third-stage column is washed through the DN chromatography adsorption column 19, and the effluent is collected as waste liquid;

[0096] Step 20: Use a peristaltic pump to deliver and an electromagnetic valve to select so that the third-stage eluent of the third-stage column passes through the DN chromatographic adsorption column 19; the effluent, i.e., the γ-radioactive solution of neodymium, is collected in the neodymium product collector 26; a radioactive measurement source can be prepared for test analysis.

[0097] In the above method, the actinide elements are various isotopes including uranium, plutonium and americium, and the lanthanide fission products are various isotopes including cerium, neodymium, samarium, europium and terbium.

[0098] Example 1

[0099] The radioactive sample containing actinide and lanthanide fission products is dissolved in 10 mL 2 mol / L HNO3, sodium nitrite is added, heated at 90-100 degrees, and cooled to form a solution containing actinide and lanthanide fission products. The solution is placed in the liquid storage tank 1, and its γ radioactivity spectrum is as follows: Figure 2 shown.

[0100] The flow rate of the solution containing actinide and lanthanide fission products is controlled at 1 mL / min, so that the radioactive sample containing actinide and lanthanide fission products is separated and adsorbed by the TRU or RE chromatographic adsorption column 17, wherein the TRU or RE chromatographic adsorption column 17 is A TRU or RE chromatography adsorption column is used to separate U, Pu, Am, Ce, Nd, Sm, Eu, Tb from Tc, Te, I, Ba, Ru, Rh, Nb, etc., and the effluent is collected in a waste liquid collector 28.

[0101] Use 25 mL of 2 mol / L HNO3 solution in the washing liquid storage tank 2, control the flow rate to 1.5 mL / min, and wash through the TRU or RE chromatography adsorption column 17 to achieve further separation of Mo and Tc, Te, I, Ba, Ru, Rh, Nb, etc., and the effluent is collected in the waste liquid collector 28.

[0102] Use 25mL 0.05mol / L HNO3 solution in the first eluent reservoir 3 of the first column, control the flow rate at 1.0mL / min, and pass it through the TRU or RE chromatography adsorption column 17 and HDEHP or P in sequence. 204 The chromatographic adsorption column 18 is eluted, wherein HDEHP or P 204 The chromatographic adsorption column 18 is HDEHP or P 204The chromatographic adsorption column realizes the desorption and re-adsorption of americium and lanthanide fission products, and the effluent is collected in the waste liquid collector 28.

[0103] Use 30mL of 0.05mol / L HNO3-0.1mol / L ACB solution in the second-stage eluent reservoir 4 of the first-stage column, control the flow rate to 1.0mL / min, pass through the TRU or RE chromatography adsorption column 17, and collect the effluent in the plutonium product collector 21.

[0104] Use 20mL of 1mol / L HCl-0.02mol / L HF solution in the third-stage eluent reservoir 5 of the first-stage column, control the flow rate to 1.0mL / min, pass through the TRU or RE chromatography adsorption column 17, and collect the effluent in the plutonium product collector 21, which is the radioactive measurement source of plutonium.

[0105] Use 10mL 0.1mol / L HCl-0.3mol / L HF solution in the fourth eluent reservoir 6 of the first column, control the flow rate to 1.0mL / min, pass through the TRU or RE chromatography adsorption column 17, and collect the effluent in the uranium product collector 20, which is the uranium radioactivity measurement source.

[0106] Use 25mL 0.1mol / L HNO3 solution in the first eluent reservoir 7 of the second column, control the flow rate to 1.0mL / min, and pass HDEHP or P 204 The chromatographic adsorption column 18 is washed and the effluent is collected in the waste liquid collector 28 .

[0107] Use 30 mL of 0.05 mol / L DTPA-1 mol / L lactic acid (pH 3.0) solution in the second-stage eluent reservoir 8 of the second-stage column, control the flow rate at 1.0 mL / min, and pass through HDEHP or P 204 The chromatographic adsorption column 18 is eluted to achieve separation of americium and lanthanide fission products, and the effluent is collected in the americium product collector 22, which is the radioactive measurement source of americium.

[0108] Use 40mL 0.2mol / L HNO3 solution in the third eluent reservoir 9 of the second column, control the flow rate at 1.0mL / min, and pass HDEHP or P 204 The chromatographic adsorption column 18 is eluted, and the effluent is collected in the waste liquid collector 28 .

[0109] Use 15mL 0.4mol / L HNO3 solution in the fourth eluent reservoir 10 of the second column, control the flow rate at 1.0mL / min, and pass through HDEHP or P in turn. 204 The chromatographic adsorption column 18 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 cerium and neodymium, and the effluent is collected in a waste liquid collector 28.

[0110] Use 8 mL of 0.4 mol / L HNO3 solution in the fourth eluent reservoir 10 of the second column, control the flow rate to 0.5 mL / min, and pass HDEHP or P 204 The chromatographic adsorption column 18 is eluted, and the effluent is collected in the waste liquid collector 28 .

[0111] Use 12mL 0.6mol / L HNO3 solution in the fifth eluent reservoir 11 of the second column, control the flow rate to 0.5mL / min, and pass HDEHP or P 204 The chromatographic adsorption column 18 is eluted, and the effluent is collected in the samarium product collector 25, which is the measurement source of the γ-radioactivity of samarium.

[0112] Use 6mL 0.6mol / L HNO3 solution in the fifth eluent reservoir 11 of the second column, control the flow rate to 0.5mL / min, and pass HDEHP or P 204 The chromatographic adsorption column 18 is eluted, and the effluent is collected in the waste liquid collector 28 .

[0113] Use 15mL 1.0mol / L HNO3 solution in the sixth eluent reservoir 12 of the second column, control the flow rate to 0.5mL / min, and pass HDEHP or P 204 The chromatographic adsorption column 18 is eluted, and the effluent is collected in the europium product collector 24, which is the gamma radioactive measurement source of europium.

[0114] Use 15mL 3.0mol / L HNO3 solution in the seventh stage eluent reservoir 13 of the second stage column, control the flow rate to 0.5mL / min, and pass HDEHP or P 204 The chromatographic adsorption column 18 is eluted, and the effluent is collected in the terbium product collector 23, which is the gamma radioactive measurement source of terbium.

[0115] Use 10 mL of 0.4 mol / L HNO3 solution in the first-stage eluent reservoir 14 of the third-stage column, control the flow rate to 0.5 mL / min, and elute through the DN chromatography adsorption column 19 at the same time, and collect the effluent in the waste liquid collector 28.

[0116] Use 20mL of 2.5mol / L HCl solution in the second eluent reservoir 15 of the third column to elute through the DN chromatography adsorption column 19 at a flow rate of 0.5mL / min. The effluent is collected in the cerium product collector 27, which is the γ-radioactivity measurement source of cerium.

[0117] Use 10 mL of 2.5 mol / L HCl solution in the second-stage eluent reservoir 15 of the third-stage column, control the flow rate to 0.5 mL / min, and elute through the DN chromatography adsorption column 19, and collect the effluent in the waste liquid collector 28.

[0118] Use 20mL of 1.5mol / L HCl solution in the third-stage eluent reservoir 16 of the third-stage column to elute through the DN chromatography adsorption column 19 at a flow rate of 0.5mL / min. The effluent is collected in the neodymium product collector 26, which is the measurement source of the γ-radioactivity of neodymium.

[0119] The experimentally obtained γ-radiation energy spectra of samarium, europium, terbium, cerium, and neodymium are as follows: Figure 3 , Figure 4 , Figure 5 , Figure 6 , Figure 7 The recovery rates of uranium, plutonium, americium, cerium, neodymium, samarium, europium, and terbium are 97.9%, 93.3%, 94.8%, 86.1%, 92.2%, 88.7%, 85.9%, and 94.2%, respectively. The decontamination factor between uranium, plutonium, and americium is 10 3 ~10 5 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 .

[0120] Example 2

[0121] The TRU chromatography adsorption column in Example 1 was replaced by an RE chromatography adsorption column, and the HDEHP chromatography adsorption column was replaced by a P 204 The separation process of Example 1 was repeated using a chromatography adsorption column to obtain radioactive measurement sources of uranium, plutonium, americium, cerium, neodymium, samarium, europium, terbium, etc. The recovery rates were 97.2%, 94.1%, 95.3%, 85.1%, 91.4%, 89.5%, 86.7%, and 96.4%, respectively. The decontamination factors are shown in Tables 1 and 2. It can be seen that the decontamination factor of the actinides is better than 10. 3 The decontamination factor between lanthanide fission products is 10 2 ~10 5 The decontamination factor for other fission products is 10 4 ~10 6 .

[0122] Table 1 Analysis of actinide element recovery and decontamination factor

[0123]

[0124] Table 2 Analysis of lanthanide fission product recovery and decontamination factor

[0125]

[0126]

[0127] Note: “>” indicates the lower limit was assigned because it was not detected.

Claims

1. A device for separating actinide and lanthanide fission products, characterized in that: It comprises a liquid storage tank unit, a chromatography separation unit, a waste liquid collector (28), 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 (28) or the product collection unit; The liquid storage tank unit, the chromatography separation unit, the product collection unit, and the waste liquid collector (28) are connected through 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 (28) and the product collection unit are located at the lowermost end; The liquid storage tank unit comprises a liquid storage tank (1) containing actinide and lanthanide fission product radioactive solution, a washing liquid storage tank (2), a first-stage column first-stage eluent storage tank (3), a first-stage column second-stage eluent storage tank (4), a first-stage column third-stage eluent storage tank (5), a first-stage column fourth-stage eluent storage tank (6), a second-stage column first-stage eluent storage tank (7), a second-stage column second-stage eluent storage tank (8), and a second-stage column third-stage eluent storage tank (9). A liquid tank (8), a third-stage eluent storage tank (9) for the second-stage column, a fourth-stage eluent storage tank (10) for the second-stage column, a fifth-stage eluent storage tank (11) for the second-stage column, a sixth-stage eluent storage tank (12) for the second-stage column, a seventh-stage eluent storage tank (13) for the second-stage column, a first-stage eluent storage tank (14) for the third-stage column, a second-stage eluent storage tank (15) for the third-stage column, and a third-stage eluent storage tank (16) for the third-stage column; The product collection unit comprises a uranium product collector (20), a plutonium product collector (21), an americium product collector (22), a terbium product collector (23), a europium product collector (24), a samarium product collector (25), a neodymium product collector (26), and a cerium product collector (27) located on the same horizontal plane; the product collection unit and the waste liquid collector (28) are located on the same horizontal plane; The chromatographic separation unit comprises a TRU or RE chromatographic adsorption column (17), a HDEHP or P 204 Chromatography adsorption column (18), DN chromatographic adsorption column (19).

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 (28), and the product collection unit is as follows: A radioactive solution storage tank containing actinide and lanthanide fission products (1), a washing solution storage tank (2), a first-stage column first-stage eluent storage tank (3), a first-stage column second-stage eluent storage tank (4), a first-stage column third-stage eluent storage tank (5), a first-stage column fourth-stage eluent storage tank (6), a second-stage column first-stage eluent storage tank (7), a second-stage column second-stage eluent storage tank (8), a second-stage column third-stage eluent storage tank (9), a second-stage column fourth-stage eluent storage tank (10), a second-stage column The outlets of the fifth eluent storage tank (11) of the column, the sixth eluent storage tank (12) of the second column, the seventh eluent storage tank (13) of the second column, the first eluent storage tank (14) of the third column, the second eluent storage tank (15) of the third column, and the third eluent storage tank (16) of the third column are connected to the corresponding inlet of the delivery pump (30) through the valve (31); the outlet of the delivery pump (30) is respectively connected to the TRU or RE chromatographic adsorption column (17), HDEHP or P through the valve (31). 204 The inlet of the chromatographic adsorption column (18) and the DN chromatographic adsorption column (19) are connected; the outlet of the TRU or RE chromatographic adsorption column (17) is connected to the uranium product collector (20), the plutonium product collector (21), the HDEHP or P through the valve (31). 204 The feed port of the chromatography adsorption column (18) is connected to the waste liquid collector (28); HDEHP or P 204 The discharge port of the chromatographic adsorption column (18) is respectively connected to an americium product collector (22), a terbium product collector (23), a europium product collector (24), a samarium product collector (25), an inlet of a DN chromatographic adsorption column (19) and a waste liquid collector (28) through a valve (31); the discharge port of the DN chromatographic adsorption column (19) is connected to a neodymium product collector (26), a cerium product collector (27) and a waste liquid collector (28) through a valve (31).

5. A method for separating actinide and lanthanide fission products, using any separation device according to claim 1 to 4, characterized in that: The steps include: Step 1, preparation before separation: The radioactive sample containing actinide elements and lanthanide fission products to be separated is dissolved in nitric acid, sodium nitrite is added, and the mixture is heated and cooled at 90 to 100° C. to obtain an aqueous radioactive sample containing actinide elements and lanthanide fission products; The washing and rinsing acids are dissolved in water respectively to obtain an aqueous washing liquid and an aqueous rinsing liquid; the washing and rinsing acids are one of nitric acid and hydrochloric acid, or a mixture of two of nitric acid, hydrochloric acid, hydrofluoric acid, diethylenetriaminepentaacetic acid, lactic acid, and ascorbic acid; TRU or RE resin, HDEHP or P 204 Resin and DN resin are respectively loaded into chromatographic adsorption columns to obtain TRU or RE chromatographic adsorption columns (17), HDEHP or P 204 Chromatographic adsorption column (18), DN chromatographic adsorption column (19); Step 2, adsorption of actinide and lanthanide fission products: The aqueous radioactive sample containing actinide and lanthanide fission products prepared in step 1 is placed in a radioactive solution storage tank containing actinide and lanthanide fission products (1), and the aqueous radioactive sample containing actinide and lanthanide fission products is separated and adsorbed using a TRU or RE chromatographic adsorption column (17), whereby the actinide and lanthanide fission products are adsorbed in the TRU or RE chromatographic adsorption column, and the effluent is collected in a waste liquid collector (28); Step 3, washing: Using an aqueous washing liquid, the TRU or RE chromatography adsorption column (17) is washed, and the effluent is collected in a waste liquid collector (28); Step 4, rinse: Use aqueous eluent to adsorb TRU or RE chromatography columns (17), HDEHP or P 204 The chromatographic adsorption column (18) and the DN chromatographic adsorption column (19) are eluted to obtain a gamma radioactive solution of europium, a gamma radioactive solution of terbium, a gamma radioactive solution of cerium, and a gamma radioactive solution of neodymium.

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 containing actinide elements and lanthanide fission products 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 6.0 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 eluent of the first column, the second eluent of the first column, the third eluent of the first column, the fourth 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 seventh eluent of the second column, the first eluent of the third column, the second eluent of the third column, the second eluent of the third column, and the third eluent of the third column; the aqueous eluent is placed in the corresponding eluent reservoir of the reservoir unit; The first eluent of the first column is 0.01mol / L~0.1mol / L HNO3 solution, the second eluent of the first column is 0.01mol / L~0.5mol / L HNO3 solution containing 0.01mol / L~0.1mol / L CB, the third eluent of the first column is 0.5mol / L~2mol / L HCl solution containing 0.01mol / L~0.03mol / L HF, the fourth eluent of the first column is 0.05mol / L~0.2mol / L HCl solution containing 0.1mol / L~0.4mol / L HF, the first eluent of the second column is 0.01mol / L~0.1mol / L HNO3 solution, the second eluent of the second column is 0.01mol / L~0.1mol / L HNO3 solution, the third eluent of the first column is 0.5mol / L~2mol / L HCl solution containing 0.01mol / L~0.03mol / L HF, the fourth eluent of the first column is 0.05mol / L~0.2mol / L HCl solution containing 0.1mol / L~0.4mol / L HF, 0.04mol / L~0.08mol / L DTPA in 0.5mol / L~1.5mol / L lactic acid solution, the third eluent of the second column is 0.15mol / L~0.25mol / L HNO3 solution, the fourth eluent of the second column is 0.25mol / L-0.45mol / LHNO3 solution, the fifth eluent of the second column is 0.5mol / L~0.75mol / L HNO3 solution, the sixth eluent of the second column is 0.8mol / L~2mol / L HNO3 solution, the seventh eluent of the second column is 2.5mol / L~4mol / L HNO3 solution, the first eluent of the third column is 0.3mol / L~0.5mol / L HNO3 solution, the second eluent of the third column is 2mol / L~3mol / L HCl solution, the third eluent of the third column is 0.1mol / L~1.5mol / L HCl solution.

9. The separation method according to claim 5, characterized in that: The step 4, elution, further comprises: The first column first eluent passes through the TRU or RE chromatography adsorption column (17) and HDEHP or P 204 A chromatographic adsorption column (18) is used to desorb and re-adsorb americium and lanthanide fission products, and the effluent is collected in a waste liquid collector (28); The second-stage eluent of the first-stage column passes through a TRU or RE chromatography adsorption column (17), and the effluent is collected in a plutonium product collector (21) to obtain a radioactive plutonium solution; The third-stage eluent of the first-stage column passes through a TRU or RE chromatography adsorption column (17), and the effluent is collected in a plutonium product collector (21) to obtain a radioactive plutonium solution; The fourth-stage eluent of the first-stage column passes through a TRU or RE chromatography adsorption column (17), and the effluent is collected in a uranium product collector (20) to obtain a radioactive uranium solution; The first eluent of the second column is HDEHP or P 204 The chromatographic adsorption column (18) is washed, and the effluent flows to the waste liquid collector (28); The second column second stage eluent is HDEHP or P 204 The effluent is collected in an americium product collector (22) to obtain a radioactive americium solution; The second column and the third eluent are HDEHP or P 204 The chromatographic adsorption column (18) is washed, and the effluent is collected in a waste liquid collector (28); The fourth stage eluent of the second column is successively passed through HDEHP or P 204 The chromatographic adsorption column (18) and the DN chromatographic adsorption column (19) are used to desorb and re-adsorb cerium and neodymium, and the effluent is collected in a waste liquid collector (28); The fourth stage eluent of the second column is HDEHP or P 204 The chromatographic adsorption column (18) is washed, and the effluent is collected in a waste liquid collector (28); The fifth stage eluent of the second column is HDEHP or P 204 The effluent from the chromatographic adsorption column (18) is collected in a samarium product collector (25) to obtain a samarium gamma-radioactive solution; The fifth stage eluent of the second column is HDEHP or P 204 The chromatographic adsorption column (18) is washed, and the effluent flows to the waste liquid collector (28); The sixth stage eluent of the second stage column is HDEHP or P 204 The effluent is collected into a europium product collector (24) through a chromatographic adsorption column (18) to obtain a europium gamma-radioactive solution; The seventh stage eluent of the second column is HDEHP or P 204 The effluent is collected in a terbium product collector (23) through a chromatography adsorption column (18) to obtain a terbium gamma-radioactive solution; The first-stage eluent of the third-stage column is washed through the DN chromatography adsorption column (19), and the effluent is collected in the waste liquid collector (28); The second-stage eluent of the third-stage column passes through a DN chromatography adsorption column (19), and the effluent is collected in a cerium product collector (27) to obtain a γ-radioactive solution of cerium; The second-stage eluent of the third-stage column is washed through the DN chromatography adsorption column (19), and the effluent is collected in the waste liquid collector (28); The third-stage eluent of the third-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.

10. The separation method according to claim 5, characterized in that: The actinide elements are isotopes including uranium, plutonium, and americium, and the lanthanide fission products are isotopes including cerium, neodymium, samarium, europium, and terbium.

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