CN104658627A - Solidified body used for performing glass curing process on low-medium radioactive waste and method - Google Patents
Solidified body used for performing glass curing process on low-medium radioactive waste and method Download PDFInfo
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- CN104658627A CN104658627A CN201510052689.7A CN201510052689A CN104658627A CN 104658627 A CN104658627 A CN 104658627A CN 201510052689 A CN201510052689 A CN 201510052689A CN 104658627 A CN104658627 A CN 104658627A
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- 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
- G21F9/04—Treating liquids
- G21F9/06—Processing
- G21F9/16—Processing by fixation in stable solid media
- G21F9/162—Processing by fixation in stable solid media in an inorganic matrix, e.g. clays, zeolites
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Abstract
The invention provides a preparation method of a solidified body used for performing glass curing process on a low-medium radioactive waste. The method comprises the following steps: taking the components SiO2, H3BO3, Na2CO3 and CaO as the raw materials, compounding and mixing, melting for 2.5-3 hours at the temperature of 1250 DEG C, after that, pouring the materials to a mold which is pre-heated to be 500 DEG C and molding, keeping the temperature at 500 DEG C for 0.5-1 hour, and then reducing the temperature to be room temperature at a rate of temperature fall of 0.5-1 DEG C/min, then the product can be prepared. The solidified body prepared by the invention can be used for performing glass curing process on the low-medium radioactive waste, realizing the volume reduction maximization of the solidified radioactive waste, more conforming to the value pursuit of waste minimization in radioactive waste treatment, and realizing the inorganization and stabilization of the solidified waste.
Description
Technical field
The present invention relates to the low middle level radioactive waste processing technology field of nuclear power station, particularly relate to a kind of firming body for the process of low medium level waste glass solidification and method.
Background technology
The development and utilization of nuclear energy brings huge economic benefit and social benefit to the mankind, also creates a large amount of radioactive wastes simultaneously, brings larger threat to the living environment of the mankind.Therefore, how to dispose radioactive waste safely and effectively, make it isolate with biosphere to greatest extent to have become nuclear industry, day by day urgent important topic that nuclear science faces, be the key factor affecting nuclear energy sustainable and healthy development.
To the disposal of radioactive waste, it is believed that the most rational measure first radioactive waste is cured process, then the solidification of radwaste body obtained is carried out final geological disposal.Process is effectively solidified to radioactive waste and can reach three objects: one, make liquid radiomaterial be transformed into be convenient to transport safely, store and the firming body of disposal operations; Two, by radioactive nuclide consolidation, stop that radioactive nuclide enters human biological's circle; Three, the volume of refuse is reduced.
Current curing technology has ceramic solidification, glass ceramics solidification, prosthetic graft solidification and glass solidification etc.Wherein, ceramic solidification is large to radioelement containing amount in low and intermediate level radioac, and crystal is strong relative to Vitrea thermal stability, but ceramic solidification is strong to the selectivity of radioactive element, and the major part in refuse is "dead", and waste material is very large to ceramic solidification influential effect, glass ceramics solidification can effectively solve ceramic solidification Problems existing, radioactive element major part is cured in lattice, cold refuse and on a small quantity uncured element in lattice are then cured in glass outer matrix, but this curing mode heat treatment process is comparatively complicated, is still in conceptual phase, though the geological stability of prosthetic graft solidification process firming body, chemical stability, thermal stability and Flouride-resistani acid phesphatase are all better, but its curing process is complicated, poor with the compatibility containing refuses such as high concentration sodium salts, very strong to the selectivity of element in low and intermediate level radioac, its technical requirement is very high, still be in laboratory theoretical research stage at present, and the equipment used is complicated, cost is high, in processing procedure, the consumption of material and the energy is all very large, glass solidification be after nuclear waste is concentrated evaporate to dryness with there is the mineral powders suitably formed mix, airtight storage in special storage field after glassy solids is become through high temperature sintering, it is high that this method has firming body intensity, density is good, Stability Analysis of Structures, the radioactive nuclide be cured leaching rate when water soaking is very low, thus security is high, in the country such as American-European-Japanese, oneself becomes one comparatively proven technique application, but the solidification of waste body made or volume and the excessive and high cost of weight, compatible degree is low, the deficiency of chemical form in solidification of waste body cannot be changed, irradiation stability and thermal stability poor.
Summary of the invention
Embodiment of the present invention technical matters to be solved is, a kind of firming body for the process of low medium level waste glass solidification and method are provided, can be used in carrying out glass solidification process with low and intermediate level radioac, realize subtracting of solidification of waste body and hold maximization, more agree with the value pursuing of " waste minimization " in Radwastes treatment, and improve the performance level of solidification of waste body, realize inorganization, the stabilization of solidification of waste body.
In order to solve the problems of the technologies described above, embodiments provide a kind of preparation method of the firming body for the process of low and intermediate level radioac glass solidification, described method comprises:
A, batching: main with component SiO
2, H
3bO
3, Na
2cO
3, CaO is raw material, and presses SiO
255 ~ 65 weight portions, H
3bO
314 ~ 21 weight portions, Na
2cO
3the ratio of 14 ~ 21 weight portions, CaO 8 ~ 12 weight portion takes each raw material;
B, mixing: each raw material is put into mixing apparatus and mixes, make mixture;
C, melting: described mixture is founded 2.5 ~ 3 hours at 1250 DEG C of constant temperature, obtained molten mass;
D, shaping: described molten mass to be poured into the die for molding being preheated to 500 DEG C, obtained article shaped;
E, annealing: be incubated 0.5 ~ 1 hour under described article shaped being placed in the temperature of 500 DEG C, be then down to room temperature with the rate of temperature fall of 0.5 ~ 1 DEG C/min, i.e. obtained product.
Wherein, Al can also be added with in described step a batching
2o
3, its adding proportion is no more than 6 weight portions.
Wherein, Fe can also be added with in described step a batching
2o
3, its adding proportion is no more than 2 weight portions.
Wherein, SO can also be added with in described step a batching
3, its adding proportion is no more than 4 weight portions.
Wherein, can also be added with MgO in described step a batching, its adding proportion is no more than 3 weight portions.
Wherein, can also be added with ZnO in described step a batching, its adding proportion is no more than 3 weight portions.
Wherein, mixing apparatus described in described step b is ball milling mixing apparatus.
Wherein, heat described in described step c and carry out under the condition stirred.
Wherein, melt cast described in described steps d is carried out under the condition of clarification homogenizing.
The embodiment of the present invention additionally provides a kind of firming body for the process of low and intermediate level radioac glass solidification, and described firming body adopts aforesaid preparation method to be prepared from.
Implement the embodiment of the present invention, there is following beneficial effect:
(1) the borosilicate glass system selected by the present invention has the feature of chemical stability, irradiation stability, good endurance, and prepared firming body is static immersing in 90 DEG C of deionized waters, and the leaching rate of Si, B, Na, Ca is much smaller than 1g/ (m
2d), weight-loss ratio is less than 15g/m
2;
(2) target glass selected by the present invention can be widely used in the multiple technologies refuse that nuclear power station produces, and makes full use of the own chemical composition of various refuse, and the maximization being conducive to waste minimization realizes, and has and subtracts appearance, weight loss effect significantly;
(3) gained formula of the present invention has the low feature of glass melting temperature, good economy performance, be easy to through engineering approaches application.
Accompanying drawing explanation
In order to be illustrated more clearly in the embodiment of the present invention or technical scheme of the prior art, be briefly described to the accompanying drawing used required in embodiment or description of the prior art below, apparently, accompanying drawing in the following describes is only some embodiments of the present invention, for those of ordinary skill in the art, under the prerequisite not paying creative work, the accompanying drawing obtaining other according to these accompanying drawings still belongs to category of the present invention.
The process flow diagram of the preparation method of the firming body for the process of low and intermediate level radioac glass solidification that Fig. 1 provides for the embodiment of the present invention one.
Embodiment
For making the object, technical solutions and advantages of the present invention clearly, below in conjunction with accompanying drawing, the present invention is described in further detail.
As shown in Figure 1, be the preparation method of a kind of firming body for the process of low and intermediate level radioac glass solidification that the embodiment of the present invention one provides, described method comprises:
A, batching: main with component SiO
2, H
3bO
3, Na
2cO
3, CaO is raw material, and presses SiO
255 ~ 65 weight portions, H
3bO
314 ~ 21 weight portions, Na
2cO
3the ratio of 14 ~ 21 weight portions, CaO 8 ~ 12 weight portion takes each raw material;
B, mixing: each raw material is put into mixing apparatus (mortar or ball-grinding machine) and mix, make mixture;
C, melting: mixture is founded 2.5 ~ 3 hours at 1250 DEG C of constant temperature, obtained molten mass;
D, shaping: molten mass to be poured into the die for molding being preheated to 500 DEG C, obtained article shaped;
E, annealing: be incubated 0.5 ~ 1 hour under article shaped being placed in the temperature of 500 DEG C, be then down to room temperature with the rate of temperature fall of 0.5 ~ 1 DEG C/min, i.e. obtained product-firming body (target glass).
Wherein, Al can also be added with in described step a batching
2o
3, its adding proportion is no more than 6 weight portions.
Wherein, Fe can also be added with in described step a batching
2o
3, its adding proportion is no more than 2 weight portions.
Wherein, SO can also be added with in described step a batching
3, its adding proportion is no more than 4 weight portions.
Wherein, can also be added with MgO in described step a batching, its adding proportion is no more than 3 weight portions.
Wherein, can also be added with ZnO in described step a batching, its adding proportion is no more than 3 weight portions.
Wherein, in described step b, mixing apparatus is ball milling mixing apparatus.
Wherein, heat in described step c and carry out as the best under the condition stirred.
Wherein, in described steps d, melt cast is carried out as the best under the condition of clarification homogenizing.
It should be noted that the component raw material in step a batching can add Al
2o
3, Fe
2o
3, SO
3, one or more combinations in MgO and ZnO, can also be can be decomposed into SiO under melt temperature
2, B
2o
3, Na
2o and/or CaO and do not introduce other starting material of impurity.In step b, mixing apparatus also can be other mixing apparatus of the prior art.
As an example 1, for the preparation method of the firming body of low and intermediate level radioac glass solidification process, described method comprises:
A, batching: main with component SiO
2, H
3bO
3, Na
2cO
3, CaO is raw material, and presses SiO
258g, H
3bO
317g, Na
2cO
3the ratio of 14g, CaO 11g takes each raw material;
B, mixing: each raw material is put into mixing apparatus (mortar or ball-grinding machine) and mix, make mixture;
C, melting: loaded by mixture in 100mL corundum crucible, send into and be preheated in the chamber type electric resistance furnace of 1250 DEG C, found 2.5 hours at 1250 DEG C, obtained molten mass;
D, shaping: molten mass to be poured in the graphite-pipe being preheated to 500 DEG C shaping, obtained article shaped;
E, annealing: the above-mentioned graphite-pipe that article shaped is housed is placed in the annealing furnace inside holding 0.5 hour being preheated to 500 DEG C, is then down to room temperature with the rate of temperature fall of 1 DEG C/min, i.e. obtained product-firming body (target glass).
As an example 2, for the preparation method of the firming body of low and intermediate level radioac glass solidification process, described method comprises:
A, batching: main with component SiO
2, H
3bO
3, Na
2cO
3, CaO, Al
2o
3for raw material, and press SiO
258g, H
3bO
315g, Na
2cO
314g, CaO 9g, Al
2o
3the ratio of 4g takes each raw material;
B, mixing: each raw material is put into mixing apparatus (mortar or ball-grinding machine) and mix, make mixture;
C, melting: loaded by mixture in 100mL corundum crucible, send into and be preheated in the chamber type electric resistance furnace of 1250 DEG C, found 2.5 hours at 1250 DEG C, obtained molten mass;
D, shaping: molten mass to be poured in the graphite-pipe being preheated to 500 DEG C shaping, obtained article shaped;
E, annealing: the above-mentioned graphite-pipe that article shaped is housed is placed in the annealing furnace inside holding 0.5 hour being preheated to 500 DEG C, is then down to room temperature with the rate of temperature fall of 1 DEG C/min, i.e. obtained product-firming body (target glass).
As an example 3, for the preparation method of the firming body of low and intermediate level radioac glass solidification process, described method comprises:
A, batching: main with component SiO
2, H
3bO
3, Na
2cO
3, CaO, Al
2o
3for raw material, and press SiO
256g, H
3bO
315g, Na
2cO
314g, CaO 9g, Al
2o
3the ratio of 4g, MgO 2g takes each raw material;
B, mixing: each raw material is put into mixing apparatus (mortar or ball-grinding machine) and mix, make mixture;
C, melting: loaded by mixture in 100mL corundum crucible, send into and be preheated in the chamber type electric resistance furnace of 1250 DEG C, found 2.5 hours at 1250 DEG C, obtained molten mass;
D, shaping: molten mass to be poured in the graphite-pipe being preheated to 500 DEG C shaping, obtained article shaped;
E, annealing: the above-mentioned graphite-pipe that article shaped is housed is placed in the annealing furnace inside holding 0.5 hour being preheated to 500 DEG C, is then down to room temperature with the rate of temperature fall of 1 DEG C/min, i.e. obtained product-firming body (target glass).
As an example 4, for the preparation method of the firming body of low and intermediate level radioac glass solidification process, described method comprises:
A, batching: main with component SiO
2, H
3bO
3, Na
2cO
3, CaO, Al
2o
3for raw material, and press SiO
256g, H
3bO
315g, Na
2cO
314g, CaO 9g, Al
2o
3the ratio of 2g, MgO 2g, ZnO 2g takes each raw material;
B, mixing: each raw material is put into mixing apparatus (mortar or ball-grinding machine) and mix, make mixture;
C, melting: loaded by mixture in 100mL corundum crucible, send into and be preheated in the chamber type electric resistance furnace of 1250 DEG C, found 2.5 hours at 1250 DEG C, obtained molten mass;
D, shaping: molten mass to be poured in the graphite-pipe being preheated to 500 DEG C shaping, obtained article shaped;
E, annealing: the above-mentioned graphite-pipe that article shaped is housed is placed in the annealing furnace inside holding 0.5 hour being preheated to 500 DEG C, is then down to room temperature with the rate of temperature fall of 1 DEG C/min, i.e. obtained product-firming body (target glass).
As an example 5, for the preparation method of the firming body of low and intermediate level radioac glass solidification process, described method comprises:
A, batching: main with component SiO
2, H
3bO
3, Na
2cO
3, CaO, Fe
2o
3for raw material, and press SiO
258g, H
3bO
315g, Na
2cO
316g, CaO 9g, Fe
2o
3the ratio of 2g takes each raw material;
B, mixing: each raw material is put into mixing apparatus (mortar or ball-grinding machine) and mix, make mixture;
C, melting: loaded by mixture in 100mL corundum crucible, send into and be preheated in the chamber type electric resistance furnace of 1250 DEG C, found 2.5 hours at 1250 DEG C, obtained molten mass;
D, shaping: molten mass to be poured in the graphite-pipe being preheated to 500 DEG C shaping, obtained article shaped;
E, annealing: the above-mentioned graphite-pipe that article shaped is housed is placed in the annealing furnace inside holding 0.5 hour being preheated to 500 DEG C, is then down to room temperature with the rate of temperature fall of 1 DEG C/min, i.e. obtained product-firming body (target glass).
Relative to the preparation method of the firming body for the process of low and intermediate level radioac glass solidification of the embodiment of the present invention one, the embodiment of the present invention two provides a kind of firming body for the process of low and intermediate level radioac glass solidification, this firming body adopts the preparation method of the embodiment of the present invention one to be prepared from, the detail of preparation method refers to the embodiment of the present invention one, and this is no longer going to repeat them.
Implement the embodiment of the present invention, there is following beneficial effect:
(1) the borosilicate glass system selected by the present invention has the feature of chemical stability, irradiation stability, good endurance, and prepared firming body is static immersing in 90 DEG C of deionized waters, and the leaching rate of Si, B, Na, Ca is much smaller than 1g/ (m
2d), weight-loss ratio is less than 15g/m
2;
(2) target glass selected by the present invention can be widely used in the multiple technologies refuse that nuclear power station produces, and makes full use of the own chemical composition of various refuse, and the maximization being conducive to waste minimization realizes, and has and subtracts appearance, weight loss effect significantly;
(3) gained formula of the present invention has the low feature of glass melting temperature, good economy performance, be easy to through engineering approaches application.
Above disclosedly be only a kind of preferred embodiment of the present invention, certainly can not limit the interest field of the present invention with this, therefore according to the equivalent variations that the claims in the present invention are done, still belong to the scope that the present invention is contained.
Claims (10)
1. for a preparation method for the firming body of low and intermediate level radioac glass solidification process, it is characterized in that, described method comprises:
A, batching: main with component SiO
2, H
3bO
3, Na
2cO
3, CaO is raw material, and presses SiO
255 ~ 65 weight portions, H
3bO
314 ~ 21 weight portions, Na
2cO
3the ratio of 14 ~ 21 weight portions, CaO 8 ~ 12 weight portion takes each raw material;
B, mixing: each raw material is put into mixing apparatus and mixes, make mixture;
C, melting: described mixture is founded 2.5 ~ 3 hours at 1250 DEG C of constant temperature, obtained molten mass;
D, shaping: described molten mass to be poured into the die for molding being preheated to 500 DEG C, obtained article shaped;
E, annealing: be incubated 0.5 ~ 1 hour under described article shaped being placed in the temperature of 500 DEG C, be then down to room temperature with the rate of temperature fall of 0.5 ~ 1 DEG C/min, i.e. obtained product.
2. preparation method as claimed in claim 1, is characterized in that, can also be added with Al in described step a batching
2o
3, its adding proportion is no more than 6 weight portions.
3. preparation method as claimed in claim 1, is characterized in that, can also be added with Fe in described step a batching
2o
3, its adding proportion is no more than 2 weight portions.
4. preparation method as claimed in claim 1, is characterized in that, can also be added with SO in described step a batching
3, its adding proportion is no more than 4 weight portions.
5. the preparation method according to any one of Claims 1-4, is characterized in that, can also be added with MgO in described step a batching, its adding proportion is no more than 3 weight portions.
6. the preparation method according to any one of Claims 1-4, is characterized in that, can also be added with ZnO in described step a batching, its adding proportion is no more than 3 weight portions.
7. preparation method as claimed in claim 1, it is characterized in that, mixing apparatus described in described step b is ball milling mixing apparatus.
8. preparation method as claimed in claim 1, is characterized in that, heat and carry out under the condition stirred described in described step c.
9. preparation method as claimed in claim 1, is characterized in that, melt cast described in described steps d is carried out under the condition of clarification homogenizing.
10. for a firming body for low and intermediate level radioac glass solidification process, it is characterized in that, described firming body adopts preparation method as claimed in any one of claims 1-9 wherein to be prepared from.
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|---|---|---|---|
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| CN104658627B CN104658627B (en) | 2017-09-01 |
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| CN105741899A (en) * | 2016-02-25 | 2016-07-06 | 中国核动力研究设计院 | Solidification treatment additive, solidification formula and solidification process for radioactive boron-containing waste liquor |
| CN106875997A (en) * | 2017-01-19 | 2017-06-20 | 杨红波 | The low technique for putting degradable waste in a kind for the treatment of |
| CN109903875A (en) * | 2019-02-28 | 2019-06-18 | 西南科技大学 | A kind of method for solidifying boron-containing nuclear waste liquid by phosphate polymer |
| CN109961868A (en) * | 2019-03-21 | 2019-07-02 | 西南科技大学 | A radioactive pollution graphite incineration process |
| CN109994240A (en) * | 2017-12-31 | 2019-07-09 | 中国人民解放军63653部队 | The method for reducing radionuclide contamination sand glass solidification fusion temperature |
| CN112551889A (en) * | 2020-12-02 | 2021-03-26 | 中广核研究院有限公司 | Glass matrix composition of lead-boron-polyethylene, glass solidified body and preparation method thereof |
| CN114068058A (en) * | 2021-11-11 | 2022-02-18 | 中广核研究院有限公司 | Method for melt processing radioactive waste |
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| CN109994240B (en) * | 2017-12-31 | 2022-10-28 | 中国人民解放军63653部队 | Method for reducing solidifying and melting temperature of radionuclide-polluted sandy soil glass |
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| CN114068058B (en) * | 2021-11-11 | 2024-03-19 | 中广核研究院有限公司 | Method for melting radioactive waste |
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| CN104658627B (en) | 2017-09-01 |
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