CN112961983A - Solution and method for extracting radionuclide from high-level vitreous body - Google Patents
Solution and method for extracting radionuclide from high-level vitreous body Download PDFInfo
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- 238000000034 method Methods 0.000 title claims abstract description 51
- 210000004127 vitreous body Anatomy 0.000 title claims abstract description 22
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims abstract description 76
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims abstract description 38
- 229910017604 nitric acid Inorganic materials 0.000 claims abstract description 38
- 239000000843 powder Substances 0.000 claims abstract description 33
- 238000002386 leaching Methods 0.000 claims description 32
- 239000007788 liquid Substances 0.000 claims description 31
- 239000007787 solid Substances 0.000 claims description 16
- 229910052792 caesium Inorganic materials 0.000 claims description 14
- 230000004992 fission Effects 0.000 claims description 7
- 229910052693 Europium Inorganic materials 0.000 claims description 3
- 238000011534 incubation Methods 0.000 claims description 3
- 229910052712 strontium Inorganic materials 0.000 claims description 3
- 229910052688 Gadolinium Inorganic materials 0.000 claims description 2
- 239000002245 particle Substances 0.000 claims description 2
- 239000011521 glass Substances 0.000 abstract description 56
- 238000000605 extraction Methods 0.000 abstract description 13
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 abstract description 9
- 239000002699 waste material Substances 0.000 abstract description 9
- 239000003513 alkali Substances 0.000 abstract description 7
- 238000009377 nuclear transmutation Methods 0.000 abstract description 7
- 230000004927 fusion Effects 0.000 abstract description 4
- 230000007797 corrosion Effects 0.000 abstract description 3
- 238000005260 corrosion Methods 0.000 abstract description 3
- 238000005516 engineering process Methods 0.000 abstract description 3
- 239000000243 solution Substances 0.000 description 24
- 239000000203 mixture Substances 0.000 description 18
- 239000011259 mixed solution Substances 0.000 description 15
- 238000005119 centrifugation Methods 0.000 description 14
- 238000001816 cooling Methods 0.000 description 14
- 238000002474 experimental method Methods 0.000 description 14
- 238000010438 heat treatment Methods 0.000 description 14
- 238000001095 inductively coupled plasma mass spectrometry Methods 0.000 description 14
- 230000002285 radioactive effect Effects 0.000 description 14
- 239000006228 supernatant Substances 0.000 description 14
- 238000007598 dipping method Methods 0.000 description 13
- 230000000052 comparative effect Effects 0.000 description 12
- 230000008569 process Effects 0.000 description 11
- 239000000047 product Substances 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- 229910052768 actinide Inorganic materials 0.000 description 4
- 150000001255 actinides Chemical class 0.000 description 4
- 239000005388 borosilicate glass Substances 0.000 description 4
- 239000002927 high level radioactive waste Substances 0.000 description 3
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 2
- CFOAUMXQOCBWNJ-UHFFFAOYSA-N [B].[Si] Chemical compound [B].[Si] CFOAUMXQOCBWNJ-UHFFFAOYSA-N 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 239000012530 fluid Substances 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 238000007496 glass forming Methods 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- 238000007500 overflow downdraw method Methods 0.000 description 2
- 238000004088 simulation Methods 0.000 description 2
- 239000002915 spent fuel radioactive waste Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 229910052695 Americium Inorganic materials 0.000 description 1
- KOPBYBDAPCDYFK-UHFFFAOYSA-N Cs2O Inorganic materials [O-2].[Cs+].[Cs+] KOPBYBDAPCDYFK-UHFFFAOYSA-N 0.000 description 1
- 229910052685 Curium Inorganic materials 0.000 description 1
- 241000282414 Homo sapiens Species 0.000 description 1
- FUJCRWPEOMXPAD-UHFFFAOYSA-N Li2O Inorganic materials [Li+].[Li+].[O-2] FUJCRWPEOMXPAD-UHFFFAOYSA-N 0.000 description 1
- KKCBUQHMOMHUOY-UHFFFAOYSA-N Na2O Inorganic materials [O-2].[Na+].[Na+] KKCBUQHMOMHUOY-UHFFFAOYSA-N 0.000 description 1
- 229910052781 Neptunium Inorganic materials 0.000 description 1
- 208000019155 Radiation injury Diseases 0.000 description 1
- 229910019603 Rh2O3 Inorganic materials 0.000 description 1
- 229910018162 SeO2 Inorganic materials 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 229910052593 corundum Inorganic materials 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- AKUNKIJLSDQFLS-UHFFFAOYSA-M dicesium;hydroxide Chemical compound [OH-].[Cs+].[Cs+] AKUNKIJLSDQFLS-UHFFFAOYSA-M 0.000 description 1
- XUCJHNOBJLKZNU-UHFFFAOYSA-M dilithium;hydroxide Chemical compound [Li+].[Li+].[OH-] XUCJHNOBJLKZNU-UHFFFAOYSA-M 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
- 238000010828 elution Methods 0.000 description 1
- YQGOJNYOYNNSMM-UHFFFAOYSA-N eosin Chemical compound [Na+].OC(=O)C1=CC=CC=C1C1=C2C=C(Br)C(=O)C(Br)=C2OC2=C(Br)C(O)=C(Br)C=C21 YQGOJNYOYNNSMM-UHFFFAOYSA-N 0.000 description 1
- 238000005530 etching Methods 0.000 description 1
- 238000009375 geological disposal Methods 0.000 description 1
- 239000000156 glass melt Substances 0.000 description 1
- -1 la2O3 Chemical class 0.000 description 1
- 229910052747 lanthanoid Inorganic materials 0.000 description 1
- 150000002602 lanthanoids Chemical class 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 230000000116 mitigating effect Effects 0.000 description 1
- PLDDOISOJJCEMH-UHFFFAOYSA-N neodymium oxide Inorganic materials [O-2].[O-2].[O-2].[Nd+3].[Nd+3] PLDDOISOJJCEMH-UHFFFAOYSA-N 0.000 description 1
- 239000003758 nuclear fuel Substances 0.000 description 1
- 230000002085 persistent effect Effects 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000003672 processing method Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 238000012958 reprocessing Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- WOCIAKWEIIZHES-UHFFFAOYSA-N ruthenium(IV) oxide Inorganic materials O=[Ru]=O WOCIAKWEIIZHES-UHFFFAOYSA-N 0.000 description 1
- JPJALAQPGMAKDF-UHFFFAOYSA-N selenium dioxide Chemical compound O=[Se]=O JPJALAQPGMAKDF-UHFFFAOYSA-N 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 238000004017 vitrification Methods 0.000 description 1
- 229910001845 yogo sapphire Inorganic materials 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B7/00—Working up raw materials other than ores, e.g. scrap, to produce non-ferrous metals and compounds thereof; Methods of a general interest or applied to the winning of more than two metals
- C22B7/006—Wet processes
- C22B7/007—Wet processes by acid leaching
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B19/00—Selenium; Tellurium; Compounds thereof
- C01B19/02—Elemental selenium or tellurium
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B26/00—Obtaining alkali, alkaline earth metals or magnesium
- C22B26/10—Obtaining alkali metals
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B26/00—Obtaining alkali, alkaline earth metals or magnesium
- C22B26/20—Obtaining alkaline earth metals or magnesium
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B30/00—Obtaining antimony, arsenic or bismuth
- C22B30/02—Obtaining antimony
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B60/00—Obtaining metals of atomic number 87 or higher, i.e. radioactive metals
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P10/00—Technologies related to metal processing
- Y02P10/20—Recycling
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- Metallurgy (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Geology (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
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Abstract
The invention belongs to the technical field of nuclear waste treatment, and discloses a solution and a method for extracting radionuclide from high-level vitreous bodies, wherein the solution comprises hydrogen peroxide and nitric acid, the concentration of the nitric acid is 0.5-2mol/L, and each liter of the solution contains 0.5-2mL of hydrogen peroxide. A method for extracting radionuclides from high-level vitreous bodies, comprising the steps of: the radionuclide in the high-level vitreous powder is leached by adding the high-level vitreous powder into the solution of the invention as described above. Compared with the traditional high-temperature alkali fusion and hydrofluoric acid corrosion, the method provided by the invention is milder and has stronger operability. The invention is expected to promote the final treatment of nuclear waste based on advanced nuclear transmutation technology and is also expected to extract useful nuclides from vitrified waste for resource utilization. In addition, the invention can also be extended to the extraction of specific elements in glass containing specific elements in other industrial fields.
Description
Technical Field
The invention belongs to the technical field of nuclear waste treatment, and particularly relates to a solution and a method for extracting radionuclide from high-level vitreous bodies.
Background
Nuclear energy is considered to be an efficient, clean energy source, and brings great economic and ecological benefits to human beings. However, fission of nuclear fuel inevitably produces radioactive spent fuel, which in turn produces large amounts of high level spent liquid during the subsequent reprocessing of spent fuel. These high level effluents have strong and persistent radiotoxicity because they contain long-lived fission products (e.g.135Cs、79Se、93Zr、107Pd, half-life greater than 105Year) and minor actinides (Am, Cm, Np). Currently, high level waste fluids are immobilized in glass matrices to prevent their migration to the environment. Among glass matrices, borosilicate glass is widely accepted as the first choice because of its high containment capacity for radionuclides and extremely high chemical durability. However, high-level waste vitrification is an expedient, far from ideal solution, because the presence of highly radioactive long-lived fissile nuclides and minor actinides in high-level vitrified bodies poses many uncertain risks to long-term geological disposal.
As an alternative, the advent of innovative nuclear transmutation techniques has indeed provided eosin for mitigating the nuclear waste problem, as it can effectively achieve a reduction in the radioactivity and half-life of long-lived fissile nuclides and minor actinides, and even a resource utilization thereof. However, it should be noted that nuclear transmutation research is still in the initial stage, taking decades to become commercialized. Most of the high level waste fluids that are currently present and are produced in the near future will be solidified into vitreous bodies. However, once nuclear transmutation techniques have made a breakthrough, long-lived fissionans and minor actinides must be extracted from these high-level glass-solidified bodies as a prerequisite for nuclear transmutation. Since boron-silicon-based high-level glass-cured bodies have good chemical durability and stability, back extraction of radionuclides therefrom would be extremely challenging.
At present, there are two methods for extracting the contained substances in the glass body by dissolving glass, namely high-temperature alkali fusion and hydrofluoride glass dissolution. However, the high-temperature alkali fusion method has harsh conditions, the concentration of the alkali liquor used is extremely high, the corrosivity is strong, and the high-temperature alkali fusion method is often required to be carried out at high temperature. The hydrofluoric acid corrosion method has extremely strong corrosivity, can easily form highly corrosive volatile gas at high temperature, and needs an additional tail gas treatment process. Therefore, the two existing methods have harsh conditions and high dangerousness, and are obviously not suitable in the future extraction process of the glass solidified nuclide, so that a method with mild extraction conditions and strong radionuclide extraction capability is urgently needed for extracting the nuclide in the glass body.
Disclosure of Invention
In order to solve the problems in the prior art, the invention aims to provide a solution and a method for extracting radionuclide from high-level vitreous bodies, and the solution and the method have mild extraction conditions and strong extraction capacity on the radionuclide.
The technical scheme adopted by the invention is as follows:
a solution for extracting radionuclides from high-level vitreous bodies comprises hydrogen peroxide and nitric acid, wherein the nitric acid has a concentration of 0.5-2mol/L and contains 0.5-2mL of hydrogen peroxide per liter of the solution.
The invention also provides a method for extracting the radionuclide from the high-level vitreous body, which comprises the following steps:
the radionuclide in the high-level vitreous powder is leached by adding the high-level vitreous powder into the solution of the invention as described above.
Preferably, after the high-level vitreous body powder is added into the solution, the temperature is raised and the temperature is kept, so that the radionuclide in the high-level vitreous body powder is leached.
Preferably, the incubation temperature is 50-90 ℃.
Preferably, the holding time is 1-10 h.
Preferably, the liquid-solid ratio of the solution to the high-level vitreous powder is 20/1 mL/g.
Preferably, the particle size of the high-level vitreous powder is 100-300 μm.
Preferably, the nuclide is a fission product nuclide.
Preferably, the nuclides include Cs, Sr, Se, Te, Gd, and Eu.
The invention has the following beneficial effects:
the solution for extracting the radionuclide from the high-level radioactive vitreous body comprises hydrogen peroxide and nitric acid, and the solution can regulate the valence state of the radionuclide in the glass solidified body by utilizing the redox capability of the hydrogen peroxide and enhance the leaching capability of the nitric acid solution on the radionuclide in the glass solidified body. Wherein the concentration of nitric acid is 0.5-2mol/L, and each liter of the solution contains 0.5-2mL of hydrogen peroxide, so that compared with the common solution with extremely high concentration and extremely strong corrosivity, the solution disclosed by the invention has the advantages that the components are milder. Meanwhile, the solution can almost completely elute the main glass components and various fission products in the high-level radioactive vitreous body from the simulation glass under a mild reaction condition (the reaction temperature is below 100 ℃), so the solution has strong extraction capability on the radioactive nuclide in the high-level radioactive vitreous body.
In the method for extracting the radionuclide from the high-level vitreous body, the high-level vitreous body powder is added into the solution, so that the radionuclide in the high-level vitreous body powder can be efficiently leached. The invention is expected to promote the final treatment of nuclear waste based on advanced nuclear transmutation technology and is also expected to extract useful nuclides from vitrified waste for resource utilization. In addition, the invention can also be extended to the extraction of specific elements in glass containing specific elements in other industrial fields.
Drawings
FIG. 1 is a graph showing the results of leaching behavior of the main glass component in comparative example 1 of the present invention in distilled water at 90 ℃ for 5 hours.
FIG. 2(a) is a graph showing Na leaching rate in examples 1 to 3 of the present invention; FIG. 2(b) is a graph showing the leaching rate of Cs in examples 1 to 3 of the present invention;
FIG. 3(a) is a graph showing Na leaching rate in examples 4 to 5 of the present invention; FIG. 3(b) is a graph showing the leaching rate of Cs in examples 4 to 5 of the present invention;
FIG. 4(a) is a graph showing Na leaching rate in examples 6 to 7 of the present invention; FIG. 4(b) is a graph showing the leaching rate of Cs in examples 6 to 7 of the present invention;
FIG. 5(a) is a graph showing leaching rates of main glass components in examples 8 to 9 of the present invention; FIG. 5(b) is a graph of the leaching rate of various fission products in example 8 to example 9 of the present invention;
FIG. 6(a) is a graph showing Na leaching rate in comparative examples 2 to 4 according to the present invention; FIG. 6(b) is a graph showing the leaching rate of Cs in comparative examples 2 to 4 of the present invention.
Detailed Description
The invention is further described below with reference to the accompanying drawings and examples.
The invention provides a method for extracting radionuclide from a high-level radioactive vitreous body, which utilizes hydrogen peroxide to assist a low-concentration nitric acid mixed solution to extract the radionuclide from a vitreous solidified body. For the sake of safety, the invention realizes the simulation of the process of extracting the radioactive nuclide from the high-level radioactive borosilicate glass body by obtaining the simulated high-level radioactive borosilicate glass solidified body by self-control and extracting the radioactive nuclide from the high-level radioactive borosilicate glass solidified body, and carries out chemical elution treatment on the glass solidified body. The simple hydrogen peroxide/nitric acid mixed solution of the present invention exhibits unexpected and surprising extractability to radionuclides in chemically robust simulated boron-silicon-based high-level glass bodies. Most of the glass composition and moldThe pseudoradionuclide is treated with (0.5-2) M HNO under mild conditions (below 100 deg.C)3/(0.5-2)mL H2O2The solution elutes, which is much milder than common extreme processing methods, such as high temperature alkali fusion and hydrofluoric acid etching of glass.
The specific scheme of the invention is as follows:
the invention relates to a method for extracting radionuclide from high-level vitreous body, comprising the following steps:
1) preparation of simulated high-magnification glass: using a primary glass-forming agent (comprising: SiO)2、B2O3、Na2O、Al2O3ZnO, CaO and Li2O) and various metal oxides (including: la2O3、Nd2O3、ZrO2、Cs2O、PdO、Rh2O3、RuO2And SeO2). La, Pd, Ru, Rh and Cs are respectively selected from representative nuclides of lanthanide elements, PGM and alkaline earth elements, and the detailed composition and the use amount of each component are shown in Table 1. These reagents (purchased from pharmaceutical chemicals, Inc.) were all non-radioactive and were mixed well. Glass forming agent and metal oxide powder were mixed in a 100mL alumina crucible at the composition content listed in Table 1, heated at 1450 ℃ for 2h, and then the glass melt was cooled to room temperature and crushed to 100 μm to obtain glass solidified body powder. The following examples and comparative examples of the present invention were each conducted using the glass-solidified powder.
TABLE 1
2) Adding the glass solidified body powder into hydrogen peroxide/nitric acid mixed solution with different content ratios of the total amount, wherein the addition amount of the hydrogen peroxide is 0.5-2mL, and the concentration of the nitric acid is 0.5-2mol/L. The present invention is described with respect to a liquid/solid ratio of 20/1mL/g, at which the leaching requirement is met.
3) And (3) placing the prepared solid-liquid mixture into an oven, heating to 50-90 ℃, preserving heat for 1-10h, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS.
4) The extraction efficiency of the above elements was evaluated based on the results of the leaching test, and the efficiency thereof was defined by formula (1).
The extraction efficiency of the elements in different leaching solutions is Vi/Mi×100(1)。
Wherein, ViSimulating the amount of the i-th element, M, extracted from the high-lying glass solidified body in different leaching solutionsiTo simulate the amount of the i-th element contained in the high-power glass solidified body.
Comparative example 1
The comparative example was carried out as follows:
and adding the self-made glass solidified body powder into the deionized water solution to obtain a solid-liquid mixture. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 90 ℃, preserving heat for 5 hours, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. As shown in FIG. 1, the leaching rates of the main components of the glass were all 0.05% or less.
Example 1
The process of the method for extracting the radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 1mL, and the concentration of the nitric acid is 1mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 90 ℃, preserving heat for 1h, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Referring to fig. 2(a) and 2(b), the leaching rates of Na and Cs were 97.69% and 98.37%, respectively.
Example 2
The process of the method for extracting the radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 1mL, and the concentration of the nitric acid is 1mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 50 ℃, preserving heat for 1h, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Referring to fig. 2(a) and 2(b), the leaching rates of Na and Cs were 92% and 70%, respectively.
Example 3
The process of the method for extracting the radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 1mL, and the concentration of the nitric acid is 1mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 70 ℃, preserving heat for 1h, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Referring to fig. 2(a) and 2(b), the leaching rates of Na and Cs were 95.4% and 81.4%, respectively.
Example 4
The process of the method for extracting the radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 2mL, and the concentration of the nitric acid is 1mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 90 ℃, preserving heat for 1h, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Referring to fig. 3(a) and 3(b), the leaching rates of Na and Cs were 99% and 99%, respectively.
Example 5
The process of the method for extracting the radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 0.5mL, and the concentration of the nitric acid is 1mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 90 ℃, preserving heat for 1h, and then cooling to room temperature. After the experiment was completed, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Referring to fig. 3(a) and 3(b), the leaching rates of Na and Cs were 90.7% and 90.4%, respectively.
Example 6
The process of the method for extracting the radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 1mL, and the concentration of the nitric acid is 0.5 mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 90 ℃, preserving heat for 1h, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Referring to fig. 4(a) and 4(b), the leaching rates of Na and Cs were 91.7% and 80%, respectively.
Example 7
The process of the method for extracting the radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 1mL, and the concentration of the nitric acid is 2mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 90 ℃, preserving heat for 1h, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Referring to fig. 4(a) and 4(b), the leaching rates of Na and Cs were 99.69% and 99.5%, respectively.
Example 8
The process of the method for extracting the radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 1mL, and the concentration of the nitric acid is 1mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 90 ℃, preserving heat for 3 hours, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Fig. 5(a) and 5(b) both show that the leaching rate of the elements exceeded 97%.
Example 9
The process of the method for extracting the radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 1mL, and the concentration of the nitric acid is 1mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 90 ℃, preserving heat for 10 hours, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Fig. 5(a) and 5(b) each show that the leaching rate of the elements exceeds 99%.
Comparative example 2
The comparative example of the method for extracting radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 0mL, and the concentration of the nitric acid is 1mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 90 ℃, preserving heat for 1h, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Referring to fig. 6(a) and 6(b), the leaching rates of Na and Cs were 46% and 65.9%, respectively.
Comparative example 3
The comparative example of the method for extracting radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 0mL, and the concentration of the nitric acid is 1mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 70 ℃, preserving heat for 1h, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Referring to fig. 6(a) and 6(b), the leaching rates of Na and Cs were 41.3% and 40.5%, respectively.
Comparative example 4
The comparative example of the method for extracting radionuclide from the high-level glass solidified body comprises the following steps:
adding the self-made glass solidified body powder into hydrogen peroxide/nitric acid mixed solutions with different content ratios, wherein the addition amount of the hydrogen peroxide is 0mL, and the concentration of the nitric acid is 1mol/L. The liquid/solid ratio was 20/1 mL/g. And (3) placing the prepared solid-liquid mixture into an oven, heating to 50 ℃, preserving heat for 1h, and then cooling to room temperature. After completion of the dipping experiment, the supernatant was collected by centrifugation and analyzed for element concentration by ICP-MS. Referring to fig. 6(a) and 6(b), the leaching rates of Na and Cs were 33.8% and 32.1%, respectively.
It can be seen from the above that, in the method for extracting radionuclide from the high-level radioactive glass solidified body, firstly, the valence state of the radionuclide in the glass solidified body is regulated and controlled by utilizing the redox capability of the hydrogen peroxide, and the leaching capability of the nitric acid solution to the radionuclide in the glass solidified body is enhanced. Under mild reaction conditions, the main glass components (Na, Ca, Al, Zn, etc.) and various fission products (Cs, Sr, Se, Gd, Eu, etc.) can be almost completely eluted from the mock glass. And secondly, compared with the traditional high-temperature alkali fusion and hydrofluoric acid corrosion, the adopted extraction method is milder and operable. The method is expected to promote the final treatment of the nuclear waste based on the advanced nuclear transmutation technology, and is also expected to extract useful nuclides from the vitrified waste for resource utilization. In addition, the invention can also be extended to the extraction of specific elements in glass containing the specific elements in other industrial fields.
Claims (9)
1. A solution for extracting radionuclides from high-level vitreous bodies comprising hydrogen peroxide and nitric acid, wherein the nitric acid has a concentration of 0.5 to 2mol/L and comprises 0.5 to 2mL of hydrogen peroxide per liter of said solution.
2. A method for extracting radionuclide from high-level vitreous body, which is characterized by comprising the following steps:
leaching radionuclides in high-level vitreous powder by adding the powder to a solution according to claim 1.
3. The method of claim 2 wherein the leaching of the radionuclide from the high level vitreous powder is accomplished by adding high level vitreous powder to the solution followed by temperature and holding.
4. A method for extracting radionuclides from high-level vitreous bodies as in claim 3 wherein the incubation temperature is 50-90 ℃.
5. The method of claim 4, wherein the incubation time is 1-10 hours.
6. The method of claim 2 wherein the ratio of liquid to solid of the solution to the high level vitreous powder is 20/1 mL/g.
7. The method as claimed in claim 2, wherein the high level vitreous powder has a particle size of 100-300 μm.
8. A method of extracting radionuclides from high-level vitreous as in claim 2, wherein the nuclide is a fission product nuclide.
9. The method of claim 8, wherein said nuclides include Cs, Sr, Se, Te, Gd, and Eu.
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Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH03100498A (en) * | 1989-09-14 | 1991-04-25 | Ishikawajima Harima Heavy Ind Co Ltd | Method for removing ruthenium tetraoxide |
| US20180286528A1 (en) * | 2017-03-31 | 2018-10-04 | Battelle Memorial Institute | Nuclear Reactor Assemblies, Nuclear Reactor Target Assemblies, and Nuclear Reactor Methods |
| CN109239759A (en) * | 2018-07-27 | 2019-01-18 | 国家海洋局南海环境监测中心（中国海监南海区检验鉴定中心） | A kind of method of rapid-digestion sample measurement radionuclide |
| CN109402413A (en) * | 2018-10-30 | 2019-03-01 | 中国工程物理研究院核物理与化学研究所 | The recovery method of palladium in a kind of spent fuel element fission product |
| CN109897971A (en) * | 2019-02-18 | 2019-06-18 | 西安交通大学 | A kind of additive and method extracting platinum group metal from radioactive glass solidified body |
-
2021
- 2021-01-28 CN CN202110121798.5A patent/CN112961983A/en active Pending
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH03100498A (en) * | 1989-09-14 | 1991-04-25 | Ishikawajima Harima Heavy Ind Co Ltd | Method for removing ruthenium tetraoxide |
| US20180286528A1 (en) * | 2017-03-31 | 2018-10-04 | Battelle Memorial Institute | Nuclear Reactor Assemblies, Nuclear Reactor Target Assemblies, and Nuclear Reactor Methods |
| CN109239759A (en) * | 2018-07-27 | 2019-01-18 | 国家海洋局南海环境监测中心（中国海监南海区检验鉴定中心） | A kind of method of rapid-digestion sample measurement radionuclide |
| CN109402413A (en) * | 2018-10-30 | 2019-03-01 | 中国工程物理研究院核物理与化学研究所 | The recovery method of palladium in a kind of spent fuel element fission product |
| CN109897971A (en) * | 2019-02-18 | 2019-06-18 | 西安交通大学 | A kind of additive and method extracting platinum group metal from radioactive glass solidified body |
Non-Patent Citations (1)
| Title |
|---|
| KOICHIRO TAKAO等: "Wet chemical processing for nuclear waste glass to retrieve radionuclides", 《JOURNAL OF HAZARDOUS MATERIALS》 * |
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