CN104658627B - A kind of firming body handled for low and intermediate level radioac glass solidification and method - Google Patents
A kind of firming body handled for low and intermediate level radioac glass solidification and method Download PDFInfo
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- CN104658627B CN104658627B CN201510052689.7A CN201510052689A CN104658627B CN 104658627 B CN104658627 B CN 104658627B CN 201510052689 A CN201510052689 A CN 201510052689A CN 104658627 B CN104658627 B CN 104658627B
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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
Abstract
The present invention provides a kind of preparation method of the firming body handled for low and intermediate level radioac glass solidification, and this method is with component SiO2、H3BO3、Na2CO3, CaO be raw material, through dispensing and mixing, at a temperature of 1250 DEG C after melting 2.5 ~ 3 hours, it is poured into and is pre-heated to 500 DEG C of die for molding, 0.5 ~ 1 hour is incubated at a temperature of being placed in 500 DEG C, room temperature is then down to 0.5 ~ 1 DEG C/min rate of temperature fall, that is, product is made.Firming body prepared by the present invention can be used in carrying out glass solidification processing with low and intermediate level radioac, realize that the volume reduction of solidification of waste body is maximized, more agree with Radwastes treatment the value pursuing of " waste minimization ", and realize inorganization, the stabilization of solidification of waste body.
Description
Technical field
The present invention relates to the low middle level radioactive waste processing technology field of nuclear power station, more particularly to it is a kind of be used for it is low in put
The firming body and method of injectivity waste glass solidification processing.
Background technology
The development and utilization of nuclear energy brings huge economic benefit and social benefit to the mankind, while also generating substantial amounts of
Radwaste, the living environment to the mankind brings larger threat.Therefore, how Spent Radioactive is safely and effectively disposed
Thing, makes it isolate the increasingly urgent important topic faced as nuclear industry, nuclear science with biosphere to greatest extent, is shadow
Ring the key factor of nuclear energy sustainable and healthy development.
Disposal to radwaste, it is believed that most rational measure is first to carry out radwaste at solidification
Reason, then carries out obtained solidification of radwaste body final geological disposal.Effective solidification is carried out to radwaste
Processing can reach three purposes：First, it is transformed into the radioactive substance of liquid be easy to transport safely, store and disposal operations
Firming body；2nd, radionuclide is consolidated, stops that radionuclide is enclosed into human biological；3rd, the volume of waste is reduced.
Current curing technology has ceramic solidification, glass ceramics solidification, prosthetic graft solidification and glass solidification etc..Wherein,
Ceramic solidification is big to radioactive element inclusion quantity in low and intermediate level radioac, and crystal phase is strong for the heat endurance of vitreum, but ceramics
Solidification is strong to the selectivity of radioactive element, and the "dead" waste material of major part in waste is very big to ceramic solidification influential effect；Glass
Glass ceramic solidification can effectively solve the problem of ceramic solidification is present, and radioactive element is largely cured in lattice, "dead"
Waste and a small amount of uncured element in lattice be then cured in glass outer matrix, but this curing mode is heat-treated
Process is complex, still in conceptual phase；Though the geological stability of prosthetic graft curing process firming body, chemical stability,
Heat endurance and Flouride-resistani acid phesphatase are all preferable, but its curing process is complicated, and the compatibility with the waste such as sodium salt containing high concentration is poor, right
The selectivity of element is very strong in low and intermediate level radioac, and its technical requirements is very high, laboratory theoretical research stage is still at present, and make
Equipment is complicated, cost is high, and the consumption of material and the energy is all very big in processing procedure；Glass solidification is to concentrate nuclear waste
It is evaporated and is mixed afterwards with the mineral powders suitably constituted, after is sintered at high temperature into glassy solids in special storage
Closed storage, this method has that firming body intensity is high, density is good, Stability Analysis of Structures, and the radionuclide being cured is through water logging
Leaching rate is very low during bubble, thus safe, and in the country such as American-European-Japanese, oneself turns into a kind of technology application of more maturation, but makes
Or into solidification of waste body volume and weight is excessive and cost is too high, or compatible degree is low, it is impossible to change in solidification of waste body
The deficiency of chemical form, irradiation stability and heat endurance are poor.
The content of the invention
Technical problem to be solved of the embodiment of the present invention is to be used for low medium level waste glass solidification there is provided one kind
The firming body and method of processing, can be used in carrying out glass solidification processing with low and intermediate level radioac, realize the volume reduction of solidification of waste body
Maximize, more agree with Radwastes treatment the value pursuing of " waste minimization ", and improve the performance of solidification of waste body
Level, realizes inorganization, the stabilization of solidification of waste body.
In order to solve the above-mentioned technical problem, it is used for the processing of low and intermediate level radioac glass solidification the embodiments of the invention provide one kind
Firming body preparation method, methods described includes：
A, dispensing：Mainly with component SiO2、H3BO3、Na2CO3, CaO be raw material, and by SiO255~65 parts by weight, H3BO3
14~21 parts by weight, Na2CO314~21 parts by weight, the ratio of the parts by weight of CaO 8~12 weigh each raw material；
B, mixing：Each raw material is put into mixing apparatus and is well mixed, mixed material is made；
C, melting：The mixed material is founded 2.5~3 hours in 1250 DEG C of constant temperature, molten mass is made；
D, shaping：The molten mass is poured into and is pre-heated to 500 DEG C of die for molding, article shaped is made；
E, annealing：0.5~1 hour is incubated at a temperature of the article shaped is placed in into 500 DEG C, then with 0.5~1 DEG C/min
Rate of temperature fall be down to room temperature, that is, be made product；
Wherein, melt cast is carried out under conditions of clarification homogenizing described in the step d.
Wherein, Al can also be added with the step a dispensings2O3, its adding proportion is no more than 6 parts by weight.
Wherein, Fe can also be added with the step a dispensings2O3, its adding proportion is no more than 2 parts by weight.
Wherein, SO can also be added with the step a dispensings3, its adding proportion is no more than 4 parts by weight.
Wherein, MgO can also be added with the step a dispensings, its adding proportion is no more than 3 parts by weight.
Wherein, ZnO can also be added with the step a dispensings, its adding proportion is no more than 3 parts by weight.
Wherein, mixing apparatus is ball milling mixing equipment described in the step b.
Wherein, heat and carried out under conditions of stirring described in the step c.
The embodiment of the present invention additionally provides a kind of firming body handled for low and intermediate level radioac glass solidification, the firming body
It is prepared from using foregoing preparation method.
Implement the embodiment of the present invention, have the advantages that：
(1) the borosilicate glass system selected by the present invention has the spy of chemical stability, irradiation stability, good endurance
Point, the prepared firming body static immersing in 90 DEG C of deionized waters, Si, B, Na, Ca leaching rate is much smaller than 1g/ (m2·d)、
Weight-loss ratio is less than 15g/m2；
(2) selected target glass of the invention is widely portable to the multiple technologies waste of nuclear power station generation, and fully
The chemical composition being had by oneself using various wastes, is conducive to the maximization of waste minimization to realize, is imitated with significant volume reduction, loss of weight
Really；
(3) present invention gained formula have glass melting temperature it is low the characteristics of, good economy performance, be easy to engineering application.
Brief description of the drawings
In order to illustrate more clearly about the embodiment of the present invention or technical scheme of the prior art, below will be to embodiment or existing
There is the accompanying drawing used required in technology description to be briefly described, it should be apparent that, drawings in the following description are only this
Some embodiments of invention, for those of ordinary skill in the art, without having to pay creative labor, according to
These accompanying drawings obtain other accompanying drawings and still fall within scope of the invention.
Fig. 1 is the preparation method for the firming body for being used for the processing of low and intermediate level radioac glass solidification that the embodiment of the present invention one is provided
Flow chart.
Embodiment
To make the object, technical solutions and advantages of the present invention clearer, the present invention is made into one below in conjunction with accompanying drawing
It is described in detail on step ground.
As shown in figure 1, a kind of solidification handled for low and intermediate level radioac glass solidification provided for the embodiment of the present invention one
The preparation method of body, methods described includes：
A, dispensing：Mainly with component SiO2、H3BO3、Na2CO3, CaO be raw material, and by SiO255~65 parts by weight, H3BO3
14~21 parts by weight, Na2CO314~21 parts by weight, the ratio of the parts by weight of CaO 8~12 weigh each raw material；
B, mixing：Each raw material is put into mixing apparatus (mortar or ball-grinding machine) and is well mixed, mixed material is made；
C, melting：Mixed material is founded 2.5~3 hours in 1250 DEG C of constant temperature, molten mass is made；
D, shaping：Molten mass is poured into and is pre-heated to 500 DEG C of die for molding, article shaped is made；
E, annealing：0.5~1 hour is incubated at a temperature of article shaped is placed in into 500 DEG C, then with 0.5~1 DEG C/min drop
Warm speed is down to room temperature, that is, product-firming body (target glass) is made.
Wherein, Al can also be added with the step a dispensings2O3, its adding proportion is no more than 6 parts by weight.
Wherein, Fe can also be added with the step a dispensings2O3, its adding proportion is no more than 2 parts by weight.
Wherein, SO can also be added with the step a dispensings3, its adding proportion is no more than 4 parts by weight.
Wherein, MgO can also be added with the step a dispensings, its adding proportion is no more than 3 parts by weight.
Wherein, ZnO can also be added with the step a dispensings, its adding proportion is no more than 3 parts by weight.
Wherein, mixing apparatus is ball milling mixing equipment in the step b.
Wherein, heat that to enter behavior under conditions of stirring optimal in the step c.
Wherein, in the step d melt cast to enter behavior under conditions of clarification homogenizing optimal.
It should be noted that the component raw material in step a dispensings can add Al2O3、Fe2O3、SO3, in MgO and ZnO
One or more combination, can also be can be decomposed into SiO under melting temperature2、B2O3、Na2O and/or CaO and do not introduce impurity
Other raw material.Mixing apparatus can also be other mixing apparatus of the prior art in step b.
As an example 1, for the preparation method of the firming body of low and intermediate level radioac glass solidification processing, methods described includes：
A, dispensing：Mainly with component SiO2、H3BO3、Na2CO3, CaO be raw material, and by SiO2 58g、H3BO3 17g、
Na2CO314g, CaO 11g ratio weigh each raw material；
B, mixing：Each raw material is put into mixing apparatus (mortar or ball-grinding machine) and is well mixed, mixed material is made；
C, melting：Mixed material is fitted into 100mL corundum crucibles, feeding is preheated in 1250 DEG C of chamber type electric resistance furnace,
Founded at 1250 DEG C 2.5 hours, molten mass is made；
D, shaping：Molten mass is poured into be pre-heated in 500 DEG C of graphite-pipe and is molded, article shaped is made；
E, annealing：The above-mentioned graphite-pipe equipped with article shaped is placed in and is preheated to 500 DEG C of annealing furnace inside holding 0.5 hour,
Then room temperature is down to 1 DEG C/min rate of temperature fall, that is, product-firming body (target glass) is made.
As an example 2, for the preparation method of the firming body of low and intermediate level radioac glass solidification processing, methods described includes：
A, dispensing：Mainly with component SiO2、H3BO3、Na2CO3、CaO、Al2O3For raw material, and by SiO2 58g、H3BO3
15g、Na2CO3 14g、CaO 9g、Al2O34g ratio weighs each raw material；
B, mixing：Each raw material is put into mixing apparatus (mortar or ball-grinding machine) and is well mixed, mixed material is made；
C, melting：Mixed material is fitted into 100mL corundum crucibles, feeding is preheated in 1250 DEG C of chamber type electric resistance furnace,
Founded at 1250 DEG C 2.5 hours, molten mass is made；
D, shaping：Molten mass is poured into be pre-heated in 500 DEG C of graphite-pipe and is molded, article shaped is made；
E, annealing：The above-mentioned graphite-pipe equipped with article shaped is placed in and is preheated to 500 DEG C of annealing furnace inside holding 0.5 hour,
Then room temperature is down to 1 DEG C/min rate of temperature fall, that is, product-firming body (target glass) is made.
As an example 3, for the preparation method of the firming body of low and intermediate level radioac glass solidification processing, methods described includes：
A, dispensing：Mainly with component SiO2、H3BO3、Na2CO3、CaO、Al2O3For raw material, and by SiO2 56g、H3BO3
15g、Na2CO3 14g、CaO 9g、Al2O34g, MgO 2g ratio weigh each raw material；
B, mixing：Each raw material is put into mixing apparatus (mortar or ball-grinding machine) and is well mixed, mixed material is made；
C, melting：Mixed material is fitted into 100mL corundum crucibles, feeding is preheated in 1250 DEG C of chamber type electric resistance furnace,
Founded at 1250 DEG C 2.5 hours, molten mass is made；
D, shaping：Molten mass is poured into be pre-heated in 500 DEG C of graphite-pipe and is molded, article shaped is made；
E, annealing：The above-mentioned graphite-pipe equipped with article shaped is placed in and is preheated to 500 DEG C of annealing furnace inside holding 0.5 hour,
Then room temperature is down to 1 DEG C/min rate of temperature fall, that is, product-firming body (target glass) is made.
As an example 4, for the preparation method of the firming body of low and intermediate level radioac glass solidification processing, methods described includes：
A, dispensing：Mainly with component SiO2、H3BO3、Na2CO3、CaO、Al2O3For raw material, and by SiO2 56g、H3BO3
15g、Na2CO3 14g、CaO 9g、Al2O32g, MgO 2g, ZnO 2g ratio weigh each raw material；
B, mixing：Each raw material is put into mixing apparatus (mortar or ball-grinding machine) and is well mixed, mixed material is made；
C, melting：Mixed material is fitted into 100mL corundum crucibles, feeding is preheated in 1250 DEG C of chamber type electric resistance furnace,
Founded at 1250 DEG C 2.5 hours, molten mass is made；
D, shaping：Molten mass is poured into be pre-heated in 500 DEG C of graphite-pipe and is molded, article shaped is made；
E, annealing：The above-mentioned graphite-pipe equipped with article shaped is placed in and is preheated to 500 DEG C of annealing furnace inside holding 0.5 hour,
Then room temperature is down to 1 DEG C/min rate of temperature fall, that is, product-firming body (target glass) is made.
As an example 5, for the preparation method of the firming body of low and intermediate level radioac glass solidification processing, methods described includes：
A, dispensing：Mainly with component SiO2、H3BO3、Na2CO3、CaO、Fe2O3For raw material, and by SiO2 58g、H3BO3
15g、Na2CO3 16g、CaO 9g、Fe2O32g ratio weighs each raw material；
B, mixing：Each raw material is put into mixing apparatus (mortar or ball-grinding machine) and is well mixed, mixed material is made；
C, melting：Mixed material is fitted into 100mL corundum crucibles, feeding is preheated in 1250 DEG C of chamber type electric resistance furnace,
Founded at 1250 DEG C 2.5 hours, molten mass is made；
D, shaping：Molten mass is poured into be pre-heated in 500 DEG C of graphite-pipe and is molded, article shaped is made；
E, annealing：The above-mentioned graphite-pipe equipped with article shaped is placed in and is preheated to 500 DEG C of annealing furnace inside holding 0.5 hour,
Then room temperature is down to 1 DEG C/min rate of temperature fall, that is, product-firming body (target glass) is made.
It is used for the preparation method for the firming body that low and intermediate level radioac glass solidification is handled relative to the embodiment of the present invention one, this
Inventive embodiments two provide a kind of firming body handled for low and intermediate level radioac glass solidification, and the firming body is real using the present invention
The preparation method for applying example one is prepared from, and the detail of preparation method refers to the embodiment of the present invention one, herein no longer one by one
Repeat.
Implement the embodiment of the present invention, have the advantages that：
(1) the borosilicate glass system selected by the present invention has the spy of chemical stability, irradiation stability, good endurance
Point, the prepared firming body static immersing in 90 DEG C of deionized waters, Si, B, Na, Ca leaching rate is much smaller than 1g/ (m2·d)、
Weight-loss ratio is less than 15g/m2；
(2) selected target glass of the invention is widely portable to the multiple technologies waste of nuclear power station generation, and fully
The chemical composition being had by oneself using various wastes, is conducive to the maximization of waste minimization to realize, is imitated with significant volume reduction, loss of weight
Really；
(3) present invention gained formula have glass melting temperature it is low the characteristics of, good economy performance, be easy to engineering application.
Above disclosed is only a kind of preferred embodiment of the invention, can not limit the power of the present invention with this certainly
Sharp scope, therefore the equivalent variations made according to the claims in the present invention, still belong to the scope that the present invention is covered.
Claims (9)
1. a kind of preparation method of the firming body handled for low and intermediate level radioac glass solidification, it is characterised in that methods described bag
Include：
A, dispensing：Mainly with component SiO2、H3BO3、Na2CO3, CaO be raw material, and by SiO255~65 parts by weight, H3BO3 14
~21 parts by weight, Na2CO3The ratio of 14~21 parts by weight and the parts by weight of CaO 8~12 weighs each raw material；
B, mixing：Each raw material is put into mixing apparatus and is well mixed, mixed material is made；
C, melting：The mixed material is founded 2.5~3 hours in 1250 DEG C of constant temperature, molten mass is made；
D, shaping：The molten mass is poured into and is pre-heated to 500 DEG C of die for molding, article shaped is made；
E, annealing：0.5~1 hour is incubated at a temperature of the article shaped is placed in into 500 DEG C, then with 0.5~1 DEG C/min drop
Warm speed is down to room temperature, that is, product is made；
Wherein, molten mass described in the step d is cast in progress under conditions of clarification homogenizing.
2. preparation method as claimed in claim 1, it is characterised in that Al can also be added with the step a dispensings2O3, its
Adding proportion is no more than 6 parts by weight.
3. preparation method as claimed in claim 1, it is characterised in that Fe can also be added with the step a dispensings2O3, its
Adding proportion is no more than 2 parts by weight.
4. preparation method as claimed in claim 1, it is characterised in that SO can also be added with the step a dispensings3, it adds
Plus ratio is no more than 4 parts by weight.
5. the preparation method as any one of Claims 1-4, it is characterised in that can also add in the step a dispensings
Added with MgO, its adding proportion is no more than 3 parts by weight.
6. the preparation method as any one of Claims 1-4, it is characterised in that can also add in the step a dispensings
Added with ZnO, its adding proportion is no more than 3 parts by weight.
7. preparation method as claimed in claim 1, it is characterised in that mixing apparatus is ball milling mixing described in the step b
Equipment.
8. preparation method as claimed in claim 1, it is characterised in that be melted in the bar stirred described in the step c
Carried out under part.
9. a kind of firming body handled for low and intermediate level radioac glass solidification, it is characterised in that the firming body uses such as right
It is required that the preparation method any one of 1 to 8 is prepared from.
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| CN105741899B (en) * | 2016-02-25 | 2018-01-30 | 中国核动力研究设计院 | A kind of curing process additive, curing formula and the technique of radioactivity borate waste solution |
| 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 |
| 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 |
| CN109903875A (en) * | 2019-02-28 | 2019-06-18 | 西南科技大学 | A kind of method that phosphate polymer solidifies boracic nuclear waste |
| CN109961868B (en) * | 2019-03-21 | 2022-03-15 | 西南科技大学 | Radioactive pollution graphite burning process |
| 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 |
| 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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| CN1119820C (en) * | 2000-04-07 | 2003-08-27 | 清华大学 | Glass-like body solidifying material for treating radioactive wastes and solidifying method |
| US7550645B2 (en) * | 2004-02-23 | 2009-06-23 | Geomatrix Solutions, Inc. | Process and composition for the immobilization of radioactive and hazardous wastes in borosilicate glass |
| CN101826376B (en) * | 2010-05-07 | 2013-07-31 | 西南科技大学 | Preparation method of vitrification substrate for radioactive nuclear waste |
| CN102157215B (en) * | 2011-03-16 | 2013-03-13 | 中科华核电技术研究院有限公司 | Method and device for treating radioactive wastes |
| CN202058473U (en) * | 2011-03-16 | 2011-11-30 | 中科华核电技术研究院有限公司 | Radioactive waste treatment device |
| CN102543237B (en) * | 2012-02-21 | 2014-12-24 | 浙江大学 | Glass solidified body and preparation method thereof |
| CN103265169B (en) * | 2013-05-24 | 2016-01-20 | 杭州电子科技大学 | A kind of preparation method of high radioactive nucleus waste vitrification base material |
| CN103345955B (en) * | 2013-07-02 | 2016-07-06 | 中科华核电技术研究院有限公司 | In, low-activity nuclear waste disposal apparatus |
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Effective date of registration: 20191104 Address after: 518000 Guangdong province Futian District Shangbu Road West of the city of Shenzhen Shenzhen science and technology building 15 layer (1502-1504, 1506) Patentee after: CHINA NUCLEAR POWER TECHNOLOGY RESEARCH INSTITUTE Address before: 518053 Guangdong province Futian District Shangbu Road West of the city of Shenzhen Shenzhen science and technology building 15 layer (1502-1504, 1506) Co-patentee before: China General Nuclear Power Corporation Patentee before: CHINA NUCLEAR POWER TECHNOLOGY RESEARCH INSTITUTE Co-patentee before: China wide nuclear electricity incorporated company |
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