CN117316487A - Method and system for treating waste sodium by utilizing high-temperature self-propagating process - Google Patents
Method and system for treating waste sodium by utilizing high-temperature self-propagating process Download PDFInfo
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- CN117316487A CN117316487A CN202311244856.9A CN202311244856A CN117316487A CN 117316487 A CN117316487 A CN 117316487A CN 202311244856 A CN202311244856 A CN 202311244856A CN 117316487 A CN117316487 A CN 117316487A
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- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 title claims abstract description 98
- 239000011734 sodium Substances 0.000 title claims abstract description 98
- 229910052708 sodium Inorganic materials 0.000 title claims abstract description 97
- 238000000034 method Methods 0.000 title claims abstract description 63
- 230000008569 process Effects 0.000 title claims abstract description 36
- 239000002699 waste material Substances 0.000 title claims abstract description 35
- 239000011521 glass Substances 0.000 claims abstract description 74
- 239000000376 reactant Substances 0.000 claims abstract description 33
- 239000007800 oxidant agent Substances 0.000 claims abstract description 31
- 238000000227 grinding Methods 0.000 claims abstract description 30
- 230000001590 oxidative effect Effects 0.000 claims abstract description 28
- 239000011261 inert gas Substances 0.000 claims abstract description 27
- 238000006479 redox reaction Methods 0.000 claims abstract description 26
- 239000011812 mixed powder Substances 0.000 claims abstract description 25
- 239000008247 solid mixture Substances 0.000 claims abstract description 25
- KEAYESYHFKHZAL-UHFFFAOYSA-N Sodium Chemical compound [Na] KEAYESYHFKHZAL-UHFFFAOYSA-N 0.000 claims abstract description 24
- 239000007788 liquid Substances 0.000 claims abstract description 24
- 238000000137 annealing Methods 0.000 claims abstract description 22
- 238000002844 melting Methods 0.000 claims abstract description 22
- 230000008018 melting Effects 0.000 claims abstract description 22
- 239000012298 atmosphere Substances 0.000 claims abstract description 21
- 230000000694 effects Effects 0.000 claims abstract description 21
- 230000002285 radioactive effect Effects 0.000 claims abstract description 21
- 229910001338 liquidmetal Inorganic materials 0.000 claims abstract description 18
- 229910001948 sodium oxide Inorganic materials 0.000 claims abstract description 14
- KKCBUQHMOMHUOY-UHFFFAOYSA-N sodium oxide Chemical compound [O-2].[Na+].[Na+] KKCBUQHMOMHUOY-UHFFFAOYSA-N 0.000 claims abstract description 13
- 230000009471 action Effects 0.000 claims abstract description 7
- 239000002994 raw material Substances 0.000 claims abstract description 7
- 238000002156 mixing Methods 0.000 claims abstract description 6
- 230000009467 reduction Effects 0.000 claims abstract description 5
- 238000006722 reduction reaction Methods 0.000 claims abstract description 5
- 238000006243 chemical reaction Methods 0.000 claims description 52
- 239000007789 gas Substances 0.000 claims description 18
- 238000002347 injection Methods 0.000 claims description 16
- 239000007924 injection Substances 0.000 claims description 16
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 14
- 238000003756 stirring Methods 0.000 claims description 11
- 238000001816 cooling Methods 0.000 claims description 10
- 238000010438 heat treatment Methods 0.000 claims description 10
- 239000002901 radioactive waste Substances 0.000 claims description 10
- 239000002912 waste gas Substances 0.000 claims description 9
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 3
- 229910002804 graphite Inorganic materials 0.000 claims description 3
- 239000010439 graphite Substances 0.000 claims description 3
- 239000000155 melt Substances 0.000 claims description 3
- 230000005012 migration Effects 0.000 claims description 3
- 238000013508 migration Methods 0.000 claims description 3
- 238000003801 milling Methods 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims description 3
- 238000007789 sealing Methods 0.000 claims description 3
- 239000000047 product Substances 0.000 description 20
- 238000007711 solidification Methods 0.000 description 9
- 230000008023 solidification Effects 0.000 description 9
- 239000007790 solid phase Substances 0.000 description 8
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 6
- 239000000843 powder Substances 0.000 description 6
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 239000002360 explosive Substances 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 229910052751 metal Inorganic materials 0.000 description 3
- 239000002184 metal Substances 0.000 description 3
- 229910044991 metal oxide Inorganic materials 0.000 description 3
- 239000002910 solid waste Substances 0.000 description 3
- 238000003860 storage Methods 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- 239000003513 alkali Substances 0.000 description 2
- 239000012300 argon atmosphere Substances 0.000 description 2
- 229910052810 boron oxide Inorganic materials 0.000 description 2
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 description 2
- 239000000292 calcium oxide Substances 0.000 description 2
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- JKWMSGQKBLHBQQ-UHFFFAOYSA-N diboron trioxide Chemical compound O=BOB=O JKWMSGQKBLHBQQ-UHFFFAOYSA-N 0.000 description 2
- 238000012423 maintenance Methods 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 2
- NDLPOXTZKUMGOV-UHFFFAOYSA-N oxo(oxoferriooxy)iron hydrate Chemical compound O.O=[Fe]O[Fe]=O NDLPOXTZKUMGOV-UHFFFAOYSA-N 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 230000005855 radiation Effects 0.000 description 2
- 230000009257 reactivity Effects 0.000 description 2
- 229910052814 silicon oxide Inorganic materials 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 238000005054 agglomeration Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000002826 coolant Substances 0.000 description 1
- 238000005202 decontamination Methods 0.000 description 1
- 230000003588 decontaminative effect Effects 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- NASFKTWZWDYFER-UHFFFAOYSA-N sodium;hydrate Chemical compound O.[Na] NASFKTWZWDYFER-UHFFFAOYSA-N 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000012265 solid product Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- 238000004017 vitrification Methods 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/28—Treating solids
- G21F9/30—Processing
- G21F9/301—Processing by fixation in stable solid media
- G21F9/302—Processing by fixation in stable solid media in an inorganic matrix
- G21F9/305—Glass or glass like matrix
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/28—Treating solids
- G21F9/34—Disposal of solid waste
- G21F9/36—Disposal of solid waste by packaging; by baling
Landscapes
- Engineering & Computer Science (AREA)
- Physics & Mathematics (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Environmental & Geological Engineering (AREA)
- Processing Of Solid Wastes (AREA)
Abstract
The application provides a method for treating waste sodium by utilizing a high-temperature self-propagating process, which comprises the following steps: melting radioactive sodium waste in an inert gas atmosphere to obtain liquid sodium metal; mixing liquid metal sodium with an oxidant in an inert gas atmosphere to perform oxidation-reduction reaction, oxidizing the liquid metal sodium into sodium oxide under the action of high-temperature self-propagating effect, and performing first grinding to obtain a solid mixture of the sodium oxide, the oxidant and a reduction product of the oxidant; adding glass raw materials into the solid mixture in the atmosphere of inert gas, and grinding for the second time to obtain glass reactant mixed powder; and melting and annealing the glass reactant mixed powder to obtain a glass finished product. The application also provides a system suitable for the method for treating the waste sodium by the high-temperature self-propagating process.
Description
Technical Field
At least one embodiment of the present application relates to a method of treating radioactive spent sodium, and in particular to a method of treating spent sodium using a high temperature self-propagating process.
Background
A Sodium-cooled fast neutron reactor (Sodium-cooled FastReactor, SFR), which is a fast neutron breeder reactor, and uses liquid Sodium as a coolant. During their operation, maintenance and replacement, small amounts of spent sodium are produced, which contains radionuclides as well as a range of soluble and insoluble impurities.
In the related art, the waste sodium treatment generated by a sodium-cooled fast neutron reactor is generally based on a water treatment method, and the treatment principle is that sodium hydroxide is generated by the reaction of sodium and water to reduce the activity of metallic sodium, and the reaction of sodium and water is vigorous and is not easy to control, and sodium-alkali reaction can be used for replacing sodium-water reaction to reduce the reaction severity. However, during the water treatment process, a large amount of hydrogen and heat are generated, which causes safety hazards. Meanwhile, the alkali liquor generated by the water treatment method also needs to be further treated and converted into an inert radioactive waste solidified body so as to realize the treatment and disposal of the final radioactive waste, and the whole process flow is relatively complex to implement and is suitable for treating a large amount of waste sodium.
Therefore, there is a need to find a method or apparatus for safely and efficiently disposing of radioactive spent sodium in sodium-cooled fast neutron reactors.
Disclosure of Invention
In view of the above, to solve at least one technical problem of the related art and other aspects, the present application proposes a method for treating sodium waste by using a high-temperature self-propagating process, including:
melting radioactive sodium waste in an inert gas atmosphere to obtain liquid sodium metal;
mixing liquid metal sodium with an oxidant in an inert gas atmosphere to perform oxidation-reduction reaction, oxidizing the liquid metal sodium into sodium oxide under the action of high-temperature self-propagating effect, and performing first grinding to obtain a solid mixture of the sodium oxide, the oxidant and a reduction product of the oxidant;
adding glass raw materials into the solid mixture in the atmosphere of inert gas, and grinding for the second time to obtain glass reactant mixed powder; and
and (3) melting and annealing the mixed powder of the glass reactants to obtain a glass finished product.
According to an embodiment of the present application, the method for treating sodium waste by using a high temperature self-propagating process further includes sealing a finished glass product in a container, and decontaminating with high pressure water to prevent radionuclide migration.
According to the embodiment of the application, the radioactive sodium waste and the glass finished product are stored in a vacuum inert gas atmosphere.
According to the embodiment of the application, the exhaust gas generated in the oxidation-reduction reaction and the annealing treatment is collected and purified.
According to the embodiment of the application, the residual heat of the high-temperature self-propagating effect is eliminated through water cooling circulation.
According to an embodiment of the present application, melting and annealing the glass reactant mixed powder includes placing a crucible loaded with the glass reactant mixed powder in a glass solidification device; heating the glass reactant mixed powder to a melting temperature of 1200 ℃ under the atmospheric atmosphere of normal pressure, and preserving the heat for 3 hours; and transferring the melt including the crucible and the glass reactant mixed powder to an annealing device for annealing.
In another aspect of the present application, a system for treating sodium waste using a high temperature self-propagating process is disclosed, suitable for use in the above method for treating sodium waste using a high temperature self-propagating process, comprising a sodium injection tank, a high temperature self-propagating reaction device, a grinding device, and a glass curing device. Wherein, the sodium injection tank is configured to melt the radioactive waste sodium to obtain liquid sodium metal; the high-temperature self-propagating reaction device is configured to mix liquid sodium metal with an oxidant and generate oxidation-reduction reaction, and a stable solid mixture is obtained under the action of high-temperature self-propagating effect; the milling device is configured to mill the solid mixture and the glass reactant; the glass curing device is configured to melt anneal the glass reactants to obtain a finished glass product.
According to embodiments of the present application, a high temperature self-propagating reaction device includes a housing, a mixer, and a reactor. Wherein, the sealed shell forms an inert gas environment in the shell; a mixer mounted within the housing and configured to mix liquid sodium metal with the oxidizing agent; the reactor is configured to receive the mixed liquid sodium metal and oxidant and to effect a redox reaction. Preferably, the reactor comprises a graphite crucible to withstand the heat generated by the redox reaction.
According to an embodiment of the present application, the high temperature self-propagating reaction apparatus further includes a cooling system configured to cool down the reactor.
According to an embodiment of the present application, the high temperature self-propagating reaction device further includes a stirring device configured to stir and mix the liquid sodium metal and the oxidizing agent in the mixer.
According to an embodiment of the present application, the system for treating sodium waste by using a high-temperature self-propagating process further includes: the control device is configured to control at least one of a flow rate of liquid sodium metal delivered to the reactor, a flow rate of inert gas delivered into the housing, and a rotational speed of the stirring device.
According to the embodiment of the application, the system for treating the sodium waste by utilizing the high-temperature self-propagating process further comprises a gas environment system and an exhaust gas collecting system. The gas environment system is connected with the sodium injection tank, the high-temperature self-propagating reaction device and the grinding device and is configured to vacuumize the sodium injection tank, the high-temperature self-propagating reaction device and the grinding device and introduce inert gas; the waste gas collecting system is connected with the high-temperature self-propagating reaction device and the grinding device and is used for collecting and purifying waste gas generated by the high-temperature self-propagating reaction device and the grinding device.
According to the examples of the present application, metallic sodium with strong reactivity is converted into sodium oxide with relatively stable properties by solid phase oxidation-reduction reaction under the effect of high temperature self-propagating effect, to obtain solid mixture powder of radioactive waste. The radioactive solid waste is then directed by melting to ultimately lead the glass product to a solidification process that achieves a small amount of radioactive spent sodium. In the process, under the condition of not producing flammable and explosive gas, the reaction is relatively mild, and the method is suitable for treating small batches of radioactive sodium wastes of not more than 5kg at one time.
Drawings
FIG. 1 is a flow chart of a method of treating spent sodium using a high temperature self-propagating process according to one embodiment of the present application; and
fig. 2 is a block diagram of a system for treating spent sodium using a high temperature self-propagating process according to one embodiment of the present application.
Reference numerals
1. A sodium injection tank;
2. a high temperature self-propagating reaction device;
2.1 a housing;
2.2 a mixer;
2.3 a reactor;
2.4 filling port;
2.5 stirring devices;
2.6 collectors;
2.7 a cooling system;
3. a grinding device;
4. a glass curing device;
4.1 heating furnace;
4.2 a curing reactor;
4.3 hand rocker;
4.4 a storage tank;
4.5 a heating furnace control system;
5. a gas environment system;
6. an exhaust gas collection system;
6.1 a gas capture device;
7. a control device;
Detailed Description
For the purposes of making the objects, technical solutions and advantages of the present application more apparent, the present application will be further described in detail below with reference to the accompanying drawings.
The endpoints of the ranges and any values recited in the application are not limited to the precise range or value, and are understood to include values approaching those range or value. For numerical ranges, one or more new numerical ranges may be obtained in combination with each other between the endpoints of each range, between the endpoint of each range and the individual point value, and between the individual point values, and are to be considered as specifically filed in the present application.
The terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the application. The terms "comprises," "comprising," and/or the like, as used herein, specify the presence of stated features, steps, operations, and/or components, but do not preclude the presence or addition of one or more other features, steps, operations, or components.
All terms (including technical and scientific terms) used herein have the same meaning as commonly understood by one of ordinary skill in the art unless otherwise defined. It should be noted that the terms used herein should be construed to have meanings consistent with the context of the present specification and should not be construed in an idealized or overly formal manner.
It is to be noted that unless otherwise defined, technical or scientific terms used herein should be taken in a general sense as understood by one of ordinary skill in the art to which this application belongs. If, throughout, reference is made to "first," "second," etc., the description of "first," "second," etc., is used merely for distinguishing between similar objects and not for understanding as indicating or implying a relative importance, order, or implicitly indicating the number of technical features indicated, it being understood that the data of "first," "second," etc., may be interchanged where appropriate.
The term "high temperature self-propagating process" as used herein refers to a technique for synthesizing materials by self-exothermal chemical reactions without external maintenance. In this application, it is specifically meant that a great amount of heat is released during the reaction by solid-phase oxidation-reduction reaction of active metal sodium with an oxidizing agent, and the high temperature is limited to 1300 ℃ or below to ensure that the reaction material is within tolerance. However, the solid mixture generated based on the high-temperature self-propagating process is not enough to be in the final stable form of the radioactive solid waste, so that the solid mixture obtained by the high-temperature self-propagating process is ground, melted and annealed, and the glass product is used as a guide to realize the solidification of a small amount of radioactive waste sodium.
Fig. 1 is a flow chart of a method of treating spent sodium using a high temperature self-propagating process according to one embodiment of the present application. Fig. 2 is a block diagram of a system for treating spent sodium using a high temperature self-propagating process according to one embodiment of the present application.
In one aspect of the present application, a method for treating sodium waste by using a high temperature self-propagating process is disclosed, as shown in fig. 1 and 2, mainly comprising the following steps S1 to S4:
s1: melting radioactive sodium waste in an inert gas atmosphere to obtain liquid sodium metal;
s2: mixing liquid metal sodium with an oxidant in a high-temperature self-propagating reaction device 2 under the atmosphere of inert gas to perform oxidation-reduction reaction, oxidizing the liquid metal sodium into sodium oxide under the action of high-temperature self-propagating effect, and performing first grinding in a grinding device 3 to obtain a solid mixture of the sodium oxide, the oxidant and a reduction product of the oxidant;
s3: adding glass raw materials into the solid mixture in an inert gas atmosphere, and performing secondary grinding in a grinding device 3 to obtain glass reactant mixed powder; and
s4: and (3) melting and annealing the glass reactant mixed powder in a glass solidification device 4 to obtain a glass finished product.
According to the examples of the present application, the mixing ratio of liquid sodium metal and oxidant is 1:1.2, wherein the oxidizing agent comprises iron oxide.
According to an embodiment of the present application, the glass raw material includes at least one of silicon oxide, calcium oxide, boron oxide, and aluminum oxide.
According to the embodiment of the application, the melting temperature of the radioactive sodium waste is 250 ℃, the temperature of the high-temperature self-propagating effect is below 1300 ℃, the melting temperature of the glass reactant mixed powder is 1100-1300 ℃, and the annealing treatment condition is that the temperature is kept for 3 hours at the normal pressure of 450-650 ℃.
According to the embodiment of the application, the vitrification process is greatly influenced by the agglomeration state of reactants, so that during the grinding treatment, the solid mixture of the sodium oxide, the oxidant and the reduction product of the oxidant is ground for the first time to ensure that the sodium is completely converted into the sodium oxide, and meanwhile, the solid mixture is dispersed and not agglomerated, and the powder of the solid mixture is in a micron level; the glass reactants are ground for the first time to be mixed uniformly.
According to the examples of the present application, metallic sodium with strong reactivity is converted into sodium oxide with relatively stable properties by solid phase oxidation-reduction reaction under the effect of high temperature self-propagating effect, to obtain solid mixture powder of radioactive waste. The radioactive solid waste is then directed by melting to ultimately lead the glass product to a solidification process that achieves a small amount of radioactive spent sodium. In the process, under the condition of not producing flammable and explosive gas, the reaction is relatively mild, and the method is suitable for treating small batches of radioactive sodium wastes of not more than 5kg at one time.
According to an embodiment of the present application, the method for treating sodium waste by using a high-temperature self-propagating process further includes:
s5: the finished glass product is sealed in a container and decontaminated using high pressure water to prevent radionuclide migration.
According to the embodiment of the application, the glass finished product is washed by high-pressure water flow to remove the radionuclide with medium binding force, and meanwhile, long-distance operation is realized, so that the nuclear radiation danger is reduced.
According to the embodiment of the application, the radioactive sodium waste and the glass finished product are stored in a vacuum inert gas atmosphere.
According to the embodiment of the application, the radioactive sodium waste is active in nature, is easy to react when being contacted with air, and meanwhile, the waste sodium and the glass finished product have the radiation irradiation danger of nuclides, so that the waste sodium and the glass finished product need to be properly stored in the atmosphere of vacuum inert gas.
According to the embodiment of the present application, the exhaust gas generated in the oxidation-reduction reaction in step S2 and the annealing treatment in step S4 is collected and purified.
According to the embodiment of the application, the waste gas generated in the oxidation-reduction reaction in the step S2 and the annealing treatment in the step S4 comprises sodium vapor escaping due to the high-temperature reaction, and the sodium vapor is collected and purified to prevent the reaction from contacting with air, so that the safety is ensured.
According to the embodiment of the application, the residual heat of the high-temperature self-propagating effect is eliminated through water cooling circulation.
According to the embodiment of the application, in order to ensure the stability and safety of the reaction materials, the temperature of the high-temperature self-propagating effect is below 1300 ℃, and after the reaction is finished, the residual heat is removed through water cooling circulation.
According to the embodiment of the application, in step S4, the melting and annealing treatment of the glass reactant mixed powder includes the following steps S401 to S403:
s401: placing a glass reactant-loaded mixed powder crucible in a glass curing device;
s402: heating the glass reactant mixed powder to a melting temperature of 1200 ℃ under the atmospheric atmosphere of normal pressure, and preserving the heat for 3 hours;
s403: the melt including the crucible and the glass reactant mixed powder is transferred to an annealing device for annealing.
In another aspect of the present application, a system for treating sodium waste using a high temperature self-propagating process is disclosed, which is suitable for the above method for treating sodium waste using a high temperature self-propagating process, as shown in fig. 2, and includes a sodium injection tank 1, a high temperature self-propagating reaction device 2, a grinding device 3, and a glass solidifying device 4. The sodium injection tank 1 is configured to melt the radioactive waste sodium to obtain liquid sodium metal; the high-temperature self-propagating reaction device 2 is configured to mix liquid sodium metal with an oxidant and perform oxidation-reduction reaction, and a stable solid mixture is obtained under the action of high-temperature self-propagating effect; the milling device 3 is configured to mill the solid mixture and the glass reactant; the glass solidifying means 4 is configured to melt anneal the glass reactants to obtain a finished glass product.
According to the system for treating sodium waste by using the high-temperature self-propagating process, disclosed by the embodiment of the application, the sodium injection tank 1 converts the radioactive sodium waste into liquid sodium metal with single components, the solid-phase oxidation-reduction reaction is initiated through the high-temperature self-propagating effect in the high-temperature self-propagating reaction device 2 so as to convert the liquid sodium metal into solid-phase metal and metal oxide powder, the solid-phase metal and metal oxide powder are uniformly dispersed in the grinding device 3, and then the liquid sodium metal is fixed in a glass form through melting and annealing in the glass solidification device 4, so that the solidification of a small amount of radioactive sodium waste is realized under the condition of not generating flammable and explosive gas.
According to the embodiment of the application, the high-temperature self-propagating reaction device 2 comprises a shell 2.1, a mixer 2.2 and a reactor 2.3. Wherein, the sealed shell 2.1 forms an inert gas environment in the shell 2.1; a mixer 2.2 mounted within the housing 2.1 and configured to mix liquid sodium metal with an oxidizing agent; reactor 2.3 is configured to receive the mixed liquid sodium metal and oxidant, and to undergo a redox reaction,
preferably, the reactor 2.3 comprises a graphite crucible to withstand the heat generated by the redox reaction.
According to the embodiment of the application, in the high-temperature self-propagating reaction device 2, an inert gas environment is created in the shell 2.1, liquid metal sodium and an oxidant are sequentially added into the reactor 2.3, and mixed in the reactor through the mixer 2.2 to perform redox reaction, so that the liquid metal sodium is converted into stable solid sodium metal oxide, and solid products are collected by the collector 2.6.
According to an embodiment of the present application, the high temperature self-propagating reaction apparatus further includes a cooling system 2.7 configured to cool down the reactor.
According to the embodiment of the application, the temperature of the high-temperature self-propagating effect is lower than 1300 ℃, a large amount of heat can be left after the oxidation-reduction reaction is completed, the heat can be rapidly removed through the cooling system 2.7, and the safety of the system is ensured.
According to the embodiment of the application, the high-temperature self-propagating reaction device 2 further comprises a stirring device 2.5, which is configured to stir and mix the liquid metal sodium and the oxidant in the mixer 2.2.
According to the embodiment of the application, in the process of oxidation-reduction reaction, the liquid metal sodium and the oxidant are uniformly and fully mixed by the stirring device 2.5, so that the reaction rate is accelerated.
According to an embodiment of the present application, the above-mentioned system for treating sodium waste using a high temperature self-propagating process further comprises a control device 7 configured to control at least one of the flow rate of liquid metal sodium delivered to the reactor 2.3, the flow rate of inert gas delivered into the housing 2.1, and the rotational speed of the stirring device 2.5.
According to the embodiment of the application, the control system 7 is connected with the sodium injection tank 1, the high-temperature self-propagating reaction device 2 and the gas environment system 5 to control the process parameters in the system and adjust the reaction progress and the environment.
According to the embodiment of the application, the glass curing device 4 comprises a heating furnace 4.1, a curing reactor 4.2, a hand-operated rod 4.3, a storage tank 4.4 and a heating furnace control system 4.5. The glass reactant mixed powder obtained by the grinding device 3 is subjected to melting and annealing reaction by a heating furnace 4.1, the temperature is controlled by a heating furnace control system 4.5, and during the period, a hand rocker 4.3 ensures that the solidification reactor 4.2 is uniformly heated, and the obtained proportional finished product is stored by a storage tank 4.4.
According to the embodiment of the application, the system for treating sodium waste by using the high-temperature self-propagating process further comprises a gas environment system 5 and an exhaust gas collecting system 6. The gas environment system 5 is connected with the sodium injection tank 1, the high-temperature self-propagating reaction device 2 and the grinding device 3 and is configured to vacuumize the sodium injection tank 1, the high-temperature self-propagating reaction device 2 and the grinding device 3 and introduce inert gas; and the waste gas collecting system 6 is connected with the high-temperature self-propagating reaction device 2 and the grinding device 3 and is used for collecting and purifying waste gas generated by the high-temperature self-propagating reaction device 2 and the grinding device 3.
According to the embodiment of the application, the gas environment system 5 vacuumizes the environments of the sodium injection tank 1, the high-temperature self-propagating reaction device 2 and the grinding device 3 and introduces inert gas to ensure that the stable existence of the metallic sodium does not react with oxygen in the air, and meanwhile, the waste gas generated by the reaction is recycled by the waste gas collecting system 6.
It should be noted that the described embodiments are only some embodiments of the present application, and not all embodiments. Based on the embodiments herein, other embodiments may be obtained by those of ordinary skill in the art without undue burden from the present disclosure.
Examples
S1: and adding the radioactive waste sodium into the sodium injection tank 1 in the argon atmosphere, and heating to about 250 ℃ to completely melt the radioactive waste sodium to obtain liquid sodium metal.
S2: in the atmosphere of argon, the liquid metal sodium obtained in the step S1 is input into a high-temperature self-propagating reaction device 2 through a sodium metering pump, and the liquid metal sodium and ferric oxide are taken as 1:1.2, adding ferric oxide into the high-temperature self-propagating reaction device 2, and carrying out solid-phase oxidation-reduction reaction to enable the liquid metal sodium to be completely oxidized, so as to finally generate a solid mixture of sodium oxide, iron and a small amount of iron oxide. The solid mixture powder is ground to obtain micron-sized solid mixture particles. Wherein the heat generated by the solid-phase oxidation-reduction reaction is carried out by the cooling system 2.7.
S3: and (3) mixing and grinding the micron-sized solid mixture particles obtained in the step (S2) with glass raw materials uniformly in an argon atmosphere to obtain glass reactant mixed powder. Wherein the glass raw materials comprise silicon oxide, calcium oxide, boron oxide and aluminum oxide.
S4: and (3) placing the glass reactant mixed powder into a glass solidification device 4, melting the glass reactant mixed powder under the conditions of atmosphere and 1200 ℃, preserving the heat for 3 hours at the highest melting temperature, and then annealing to obtain a glass finished product.
S5: and (3) washing the glass finished product obtained in the step (S4) by high-pressure water, performing radioactive decontamination, and sealing and storing.
The foregoing embodiments have been provided for the purpose of illustrating the general principles of the present application and are not meant to limit the scope of the invention, but to limit the scope of the invention.
Claims (12)
1. A method for treating waste sodium by using a high-temperature self-propagating process, comprising:
melting radioactive sodium waste in an inert gas atmosphere to obtain liquid sodium metal;
mixing the liquid metal sodium with an oxidant in an inert gas atmosphere to perform oxidation-reduction reaction, oxidizing the liquid metal sodium into sodium oxide under the action of high-temperature self-propagating effect, and performing first grinding to obtain a solid mixture of sodium oxide, the oxidant and a reduction product of the oxidant;
adding glass raw materials into the solid mixture in the atmosphere of inert gas, and carrying out secondary grinding to obtain glass reactant mixed powder; and
and (3) melting and annealing the glass reactant mixed powder to obtain a glass finished product.
2. The method of claim 1, further comprising sealing the finished glass product in a container and decontaminating with high pressure water to prevent radionuclide migration.
3. The method of claim 1 or 2, wherein the radioactive spent sodium and the finished glass product are stored in a vacuum inert gas atmosphere.
4. The method according to claim 1 or 2, wherein the exhaust gas generated in the oxidation-reduction reaction and the annealing treatment is collected and purified.
5. The method of claim 1, wherein the remaining heat of the high temperature self-propagating effect is removed by a water cooling cycle.
6. The method of claim 1, wherein melting and annealing the glass reactant mixed powder comprises:
placing a crucible carrying the glass reactant mixed powder in a glass curing device;
heating the glass reactant mixed powder to a melting temperature of 1200 ℃ under the atmospheric atmosphere of normal pressure, and preserving heat for 3 hours; and
transferring the melt of the glass reactant mixed powder including the crucible to an annealing device for annealing.
7. A system for treating sodium waste using a high temperature self-propagating process, adapted for use in the method of any one of claims 1 to 6, comprising:
a sodium injection tank configured to melt the radioactive waste sodium to obtain liquid sodium metal;
the high-temperature self-propagating reaction device is configured to mix the liquid metal sodium with the oxidant and generate oxidation-reduction reaction, and a stable solid mixture is obtained under the action of the high-temperature self-propagating effect;
a milling device configured to mill the solid mixture and glass reactant; and
and the glass solidifying device is configured to perform melt annealing on the glass reactant to obtain a glass finished product.
8. The system of claim 7, wherein the high temperature self-propagating reaction device comprises:
a sealed housing, an inert gas environment being formed within the housing;
a mixer mounted within the housing and configured to mix the liquid sodium metal with an oxidizing agent; and
a reactor configured to receive the mixed liquid sodium metal and oxidant and to effect a redox reaction,
preferably, the reactor comprises a graphite crucible to withstand the heat generated by the redox reaction.
9. The system of claim 8, wherein the high temperature self-propagating reaction device further comprises: and a cooling system configured to cool down the reactor.
10. The system of claim 8, wherein the high temperature self-propagating reaction device further comprises: and a stirring device configured to stir and mix the liquid metal sodium and the oxidizing agent in the mixer.
11. The system of claim 10, further comprising: a control device configured to control at least one of a flow rate of the liquid sodium metal delivered to the reactor, a flow rate of an inert gas delivered into the housing, and a rotational speed of the stirring device.
12. The system of any of claims 7-11, further comprising:
the gas environment system is connected with the sodium injection tank, the high-temperature self-propagating reaction device and the grinding device and is configured to vacuumize the sodium injection tank, the high-temperature self-propagating reaction device and the grinding device and introduce inert gas; and
and the waste gas collecting system is connected with the high-temperature self-propagating reaction device and the grinding device and is used for collecting and purifying waste gas generated by the high-temperature self-propagating reaction device and the grinding device.
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