CN103680660A - Application of cullet in solidifying radionuclide and normal temperature solidifying method for waste comprising radioactive Cs+ - Google Patents
Application of cullet in solidifying radionuclide and normal temperature solidifying method for waste comprising radioactive Cs+ Download PDFInfo
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- CN103680660A CN103680660A CN201310644030.1A CN201310644030A CN103680660A CN 103680660 A CN103680660 A CN 103680660A CN 201310644030 A CN201310644030 A CN 201310644030A CN 103680660 A CN103680660 A CN 103680660A
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- cullet
- normal temperature
- waste
- refuse
- solidifying
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- 239000006063 cullet Substances 0.000 title claims abstract description 61
- 230000002285 radioactive effect Effects 0.000 title claims abstract description 37
- 238000000034 method Methods 0.000 title claims abstract description 15
- 239000002699 waste material Substances 0.000 title abstract description 11
- 238000012423 maintenance Methods 0.000 claims abstract description 14
- 239000000843 powder Substances 0.000 claims abstract description 10
- 238000001035 drying Methods 0.000 claims abstract description 7
- 238000007789 sealing Methods 0.000 claims abstract description 7
- 239000002002 slurry Substances 0.000 claims abstract description 6
- 238000002360 preparation method Methods 0.000 claims abstract description 5
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 7
- 239000012190 activator Substances 0.000 claims description 7
- 239000003795 chemical substances by application Substances 0.000 claims description 7
- AIYUHDOJVYHVIT-UHFFFAOYSA-M caesium chloride Chemical compound [Cl-].[Cs+] AIYUHDOJVYHVIT-UHFFFAOYSA-M 0.000 claims description 6
- 238000012545 processing Methods 0.000 claims description 6
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 5
- 238000000498 ball milling Methods 0.000 claims description 5
- 150000003839 salts Chemical class 0.000 claims description 5
- NLSCHDZTHVNDCP-UHFFFAOYSA-N caesium nitrate Chemical group [Cs+].[O-][N+]([O-])=O NLSCHDZTHVNDCP-UHFFFAOYSA-N 0.000 claims description 4
- 239000004111 Potassium silicate Substances 0.000 claims description 3
- 239000004115 Sodium Silicate Substances 0.000 claims description 3
- 229910052913 potassium silicate Inorganic materials 0.000 claims description 3
- NNHHDJVEYQHLHG-UHFFFAOYSA-N potassium silicate Chemical compound [K+].[K+].[O-][Si]([O-])=O NNHHDJVEYQHLHG-UHFFFAOYSA-N 0.000 claims description 3
- 235000019353 potassium silicate Nutrition 0.000 claims description 3
- 229910052911 sodium silicate Inorganic materials 0.000 claims description 3
- NTHWMYGWWRZVTN-UHFFFAOYSA-N sodium silicate Chemical compound [Na+].[Na+].[O-][Si]([O-])=O NTHWMYGWWRZVTN-UHFFFAOYSA-N 0.000 claims description 3
- 230000005284 excitation Effects 0.000 claims description 2
- 238000004519 manufacturing process Methods 0.000 claims description 2
- 238000002386 leaching Methods 0.000 abstract description 25
- 239000000463 material Substances 0.000 abstract description 7
- 239000011398 Portland cement Substances 0.000 abstract description 5
- 229910017053 inorganic salt Inorganic materials 0.000 abstract description 4
- 239000002910 solid waste Substances 0.000 abstract description 4
- 239000011159 matrix material Substances 0.000 abstract description 2
- 238000003756 stirring Methods 0.000 abstract 2
- 238000000227 grinding Methods 0.000 abstract 1
- 238000002156 mixing Methods 0.000 abstract 1
- 238000005406 washing Methods 0.000 abstract 1
- 239000000243 solution Substances 0.000 description 17
- 239000004568 cement Substances 0.000 description 11
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 10
- 238000007711 solidification Methods 0.000 description 7
- 230000008023 solidification Effects 0.000 description 7
- 230000007613 environmental effect Effects 0.000 description 5
- 239000002901 radioactive waste Substances 0.000 description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 5
- 229910000831 Steel Inorganic materials 0.000 description 4
- 239000008367 deionised water Substances 0.000 description 4
- 229910021641 deionized water Inorganic materials 0.000 description 4
- 239000011521 glass Substances 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- 239000010959 steel Substances 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 3
- 239000012266 salt solution Substances 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- 239000003643 water by type Substances 0.000 description 3
- 230000008901 benefit Effects 0.000 description 2
- 230000006835 compression Effects 0.000 description 2
- 238000007906 compression Methods 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000005025 nuclear technology Methods 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 235000011121 sodium hydroxide Nutrition 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 1
- 244000309464 bull Species 0.000 description 1
- 238000011109 contamination Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
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- Processing Of Solid Wastes (AREA)
Abstract
The invention discloses application of cullet in solidifying radionuclide and a normal temperature solidifying method for waste comprising radioactive Cs+. The solidifying process comprises the steps of washing and drying the cullet, grinding the cullet into powder through a ball grinder, adding inorganic salt comprising the waste comprising the radioactive Cs+ into an alkaline excitant, mixing and stirring the alkaline excitant with the waste comprising the radioactive Cs+ and the cullet powder into slurry, after full stirring, placing the slurry into a die for carrying out vibration to eliminate bubbles in a reaction system, finally, carrying out sealing, maintenance, releasing and drying on the die after being treated with vibration to obtain cullet matrix normal-temperature solidified body comprising the radionuclide Cs+. According to the method, compared with traditional portland cement, the solidified body prepared through the cullet is excellent in mechanical property and leaching resistance. The whole solidifying process saves energy, reduces consumption, and is good in safety. The most common solid waste, namely, the cullet is mainly utilized in preparation of solidifying materials, the waste is treated through other waste, and therefore the environment is protected.
Description
Technical field
The invention belongs to radioactive waste environmental protection treatment technical field, take cullet as the curing radioactive nuclide of curing material, develop a kind of new and effective curing radioactive nuclide Cs simultaneously
+normal temperature cure method.
Background technology
Nuclear energy and nuclear technology have obtained increasingly extensive application in fields such as industry, national defence, scientific researches.But when application nuclear technology is brought tremendous economic and social benefit to the mankind, also produced a large amount of radioactive wastes.These radioactive wastes have specific radiobiology toxicity, if be leaked to biosphere, can cause serious radioactive contamination, will the mankind and environment be caused to huge harm.
Cement is the curing technology of matrix because equipment is simple, investment and operating cost low, now become current topmost Solidification Measures of Radioactive Waste.But the characteristic that the poriness of cement solidification material and chemical stability are poor, causes the leaching rate of radioactive nuclide higher, has increased the difficulty of curing radioactive waste, has improved potential environmental risk.Therefore, research and develop novel solidification of radwaste material and become whole world question of common concern.
Summary of the invention
The technical problem to be solved in the present invention is to develop to using cullet and as curing material, solidify the new purposes of radioactive nuclide, proposes to solidify containing radioactivity Cs with cullet simultaneously
+the normal temperature cure method of refuse, this purposes has been utilized modal solid waste glass, the treatment of wastes with processes of wastes against one another, environmental protection.
First, the present invention proposes the new purposes of the application of cullet in solidifying radioactive nuclide.
In addition, the present invention proposes a kind of application cullet solidifies containing radioactivity Cs
+the normal temperature cure preparation of refuse, it comprises the following steps:.
1), by cullet cleaning-drying, ball milling powdered in bowl mill, screens through 200 mesh sieve afterwards;
2) will be containing radioactivity Cs
+the inorganic salts of refuse add in alkali-activator, then alkali-activator and cullet powder are mixed into slurry, put into mould and vibrate, to get rid of bubble contained in reaction system after reaction system is fully stirred;
3), by the mould sealing after vibration processing, maintenance, the demoulding, make containing simulated radioactive nuclein Cs after dry
+cullet base normal temperature cure body.
Above-mentioned steps 1) cullet in is the cullet producing in the municipal cullet reclaiming or commercial production.
Above-mentioned steps 2) described alkaline excitation agent solution is sodium hydroxide solution or potassium hydroxide solution, the potpourri of sodium silicate solution or potassium silicate solution or above-mentioned solution.
Above-mentioned steps 2) described radioactive nuclide Cs
+with the mass ratio of cullet be 0.5～1.5:50.
Above-mentioned steps 2) described containing radioactivity Cs
+the inorganic salts form of refuse is cesium nitrate (CsNO
3), one or more in cesium chloride (CsCl).
Beneficial effect of the present invention:
After measured, containing radioactive nuclide Cs
+the 42 day Dynamic Leaching rates of cullet normal temperature cure body in the Adlerika that sulfuric acid solution and the massfraction of 25 ℃ of deionized waters, pH=1 is 5% be respectively 2.18 * 10
-5cm/d, 3.96 * 10
-3cm/d, 8.88 * 10
-3cm/d, the 42 day Dynamic Leaching rates of solidified cement body in these three kinds of solution are respectively 1.04 * 10
-3cm/d, 1.12 * 10
-3cm/d, 1.56 * 10
-3cm/d.Thereby glass-based normal temperature cure body can effectively improve radioactive nuclide Cs
+solidification effect, reduce its leaching rate.
In sum, application cullet normal temperature cure body solidifies radioactive nuclide Cs
+compare with traditional cement solidification, have following advantage:
(1) application cullet base normal temperature cure body solidifies radioactive nuclide Cs
+, can effectively reduce radioactive nuclide Cs
+leaching rate, improve solidification effect.
(2) application cullet base normal temperature cure body solidifies radioactive nuclide Cs
+, fund input is lower, can effectively utilize the solid waste of banking up---cullet, thereby have very high practicality, the feature of environmental protection and using value simultaneously.
Accompanying drawing explanation
Fig. 1: firming body microscopic appearance (SEM) figure, wherein Fig. 1 a is solidified cement body scanning electron microscope (SEM) photograph, Fig. 1 b is cullet base normal temperature cure swept-volume Electronic Speculum figure;
Fig. 2: cullet base normal temperature cure body and solidified cement body compressive strength figure;
Fig. 3: cullet base normal temperature cure body anti-leaching design sketch; Wherein Fig. 3 a is 25 ℃ of states, and Fig. 3 b is 70 ℃ of states;
Fig. 4: solidified cement body anti-leaching design sketch, wherein Fig. 4 a is 25 ℃ of states, Fig. 4 b is 70 ℃ of states.
Embodiment
Below in conjunction with accompanying drawing, the specific embodiment of the present invention is described in further detail:
Embodiment 1
1) cullet cleaning-drying ball milling are become to glass powder, in 90 ℃ of baking ovens, dry 2h;
2) by 1.5 moles of sodium silicate solutions and containing simulated emission Cs
+inorganic salt solution (the CsNO of refuse
3with CsCl
2potpourri) mix, then alkali-activator and cullet powder are mixed, make radioactive nuclide Cs
+with the mass ratio of cullet be 1:50;
3) pour in steel three gang moulds after reaction system is fully stirred, mould is placed on electric vibration table and vibrates 5 minutes, to get rid of bubble contained in reaction system;
4) by the mould sealing after vibration processing, be placed in curing box maintenance demoulding after 24 hours at 60 ℃; Sample after the demoulding continues at 60 ℃ maintenance 28 days, makes containing radioactive nuclide Cs after dry
+cullet base normal temperature cure body.
1) cullet cleaning-drying ball milling are become to cullet powder, in 90 ℃ of baking ovens, dry 2h;
2) by 1.0 moles of potassium silicate solutions and containing simulated emission Cs
+inorganic salt solution (the CsNO of refuse
3potpourri with CsCl) mix, then alkali-activator and cullet powder are mixed, make radioactive nuclide Cs
+with the mass ratio of cullet be 1.5:50;
3) pour in steel three gang moulds after reaction system is fully stirred, mould is placed on electric vibration table and vibrates 5 minutes, to get rid of bubble contained in reaction system;
4) by the mould sealing after vibration processing, be placed in curing box maintenance demoulding after 24 hours at 60 ℃; Sample after the demoulding continues at 60 ℃ maintenance 28 days, makes containing radioactive nuclide Cs after dry
+cullet base normal temperature cure body.
1) cullet cleaning-drying ball milling are become to cullet powder, in 90 ℃ of baking ovens, dry 2h;
2) by the mixed solution of 1.0 molar sodium hydroxides and potassium hydroxide and containing simulated emission Cs
+inorganic salt solution (the Cs of refuse
2sO
4solution) mix, then make mixed liquor mix with cullet powder, make radioactive nuclide Cs
+with the mass ratio of cullet be 0.5:50;
3) pour in steel three gang moulds after reaction system is fully stirred, mould is placed on electric vibration table and vibrates 5 minutes, to get rid of bubble contained in reaction system;
4) by the mould sealing after vibration processing, be placed in curing box maintenance demoulding after 24 hours at 60 ℃; Sample after the demoulding continues at 60 ℃ maintenance 28 days, makes containing radioactive nuclide Cs after dry
+cullet base normal temperature cure body.
1) mensuration of firming body compressive property
Treat containing radioactive nuclide Cs
+the normal temperature cure of cullet base recuperate and protect to the predetermined length of time, get 3 samples, measure its compressive strength, get three's mean value as the resistance to compression value of firming body, the results are shown in Figure 2;
3) firming body anti-leaching performance measurement
(1) by maintenance to the predetermined length of time containing radioactive nuclide Cs
+cullet base normal temperature cure body be placed in respectively the sulfuric acid solution of 300ml25 ℃ of deionized water, pH=1 and the plastic bottle with cover of the Adlerika that massfraction is 5% be housed, and the plastic bottle that 25 ℃ of deionized water solutions are housed be placed in respectively to 25 ℃ of baking ovens keep constant temperature;
(2) from starting leaching test, within the 1st, 3,7,10,14,21,28,34,42 days, change leaching agent, and measure the concentration of radioactive nuclide in leaching agent, the results are shown in Figure 3.The leaching rate of radioactive nuclide Cs+ in leachate
pass with extraction time is:
In formula:
be the leaching rate of i component in n leaching cycle, cmd
-1;
be the quality of the i component that leaches in n leaching cycle, g;
for the initial mass of i component in leaching test sample, g; F is the geometric area that sample contacts with leaching agent, cm
2; V is the volume of sample, cm
3; t
nbe the continuous days of n leaching cycle, d;
4) contrast experiment
Portland cement and suitable quantity of water are mixed into slurry, then will be containing simulated emission Cs
+the inorganic salts of refuse (solution or waste residue) add in cement slurry, make radioactive nuclide Cs
+with the mass ratio of cement be 0.5～1.5:50; After reaction system is fully stirred, pour in steel three gang moulds, mould is placed on electric vibration table and vibrates 5 minutes, to get rid of bubble contained in reaction system; Mould sealing by after vibration processing, is placed in curing box maintenance demoulding after 24 hours at 60 ℃; Sample after the demoulding continues at 60 ℃ maintenance 28 days, makes containing radioactive nuclide Cs after dry
+portland cement firming body; Treat containing radioactive nuclide Cs
+the maintenance of Portland cement firming body to after the predetermined length of time, get 3 samples, measure its compressive strength, get three's mean value as the resistance to compression value of firming body, the results are shown in Figure 2; By maintenance to the predetermined length of time containing radioactive nuclide Cs
+portland cement firming body be placed in respectively the sulfuric acid solution of 300ml25 ℃ of deionized water, pH=1 and the plastic bottle with cover of the Adlerika that massfraction is 5% be housed, and the plastic bottle that 25 ℃ of deionized water solutions are housed be placed in respectively to the baking oven of 25 ℃ keep constant temperature; From starting leaching test, within the 1st, 3,7,10,14,21,28,35,42 days, change leaching agent, and measure the concentration of radioactive nuclide in leaching agent, the results are shown in Figure 4.
Comparison diagram 1a, b can find, the microscopic appearance of cullet base normal temperature cure body is more smooth, fine and close; Fig. 2 shows, firming body prepared by cullet material has good mechanical property and anti-leaching performance, and its 28 days compressive strength surpass 80MPa, apparently higher than solidified cement body; Comprehensive Correlation Fig. 3 and Fig. 4 can draw, 42 days Dynamic Leaching rates in the Adlerika that sulfuric acid solution and the massfraction of 25 ℃ of deionized waters, pH=1 is 5% are respectively 2.18 * 10
-5cm/d, 3.96 * 10
-3cm/d, 8.88 * 10
-3well below solidified cement body, 42 days Dynamic Leaching rates in the Adlerika that sulfuric acid solution and the massfraction of 25 ℃ of deionized waters, pH=1 is 5% (are respectively 1.04 * 10 to cm/d
-3cm/d, 1.12 * 10
-3cm/d, 1.56 * 10
-3cm/d).And whole solidification process is without through complicated processes such as compressing tablet, high temperature sintering, collosol and gel pre-service repeatedly, so this energy saving technology consumption reduction, security are good.And the preparation of curing materials has mainly utilized modal solid waste glass, the treatment of wastes with processes of wastes against one another, environmental protection.
Claims (6)
1. the application of cullet in solidifying radioactive nuclide.
2. an application cullet solidifies containing radioactivity Cs
+the normal temperature cure method of refuse, is characterized in that, comprises the following steps:
1), by cullet cleaning-drying, ball milling powdered in bowl mill, screens through 200 object sieves afterwards;
2) will be containing radioactivity Cs
+the inorganic salts of refuse add in alkali-activator, then alkali-activator and cullet powder are mixed into slurry, put into mould and vibrate, to get rid of bubble contained in reaction system after reaction system is fully stirred;
3), by the mould sealing after vibration processing, maintenance, the demoulding, make containing simulated radioactive nuclein Cs after dry
+cullet base normal temperature cure body.
3. application cullet according to claim 2 solidifies containing radioactivity Cs
+the normal temperature cure method of refuse, is characterized in that, the cullet in step 1) is the cullet producing in the municipal cullet reclaiming or commercial production.
4. according to the application cullet described in claim 2 or 3, solidify containing radioactivity Cs
+the normal temperature cure method of refuse, is characterized in that step 2) described alkaline excitation agent solution is the potpourri of sodium hydroxide solution or potassium hydroxide solution or sodium silicate solution or potassium silicate solution or above-mentioned solution.
5. according to a kind of application cullet described in claim 2 or 3, solidify containing radioactivity Cs
+the normal temperature cure preparation of refuse, is characterized in that step 2) described radioactive nuclide Cs
+with the mass ratio of cullet be 0.5 ~ 1.5:50, the mass ratio of alkali-activator and cullet is 0.4 ~ 0.6:1.
6. according to a kind of application cullet described in claim 2 or 3, solidify containing radioactivity Cs
+the normal temperature cure preparation of refuse, is characterized in that step 2) described containing radioactivity Cs
+the inorganic salts form of refuse is cesium nitrate (CsNO
3), one or more in cesium chloride (CsCl).
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201310644030.1A CN103680660A (en) | 2013-12-03 | 2013-12-03 | Application of cullet in solidifying radionuclide and normal temperature solidifying method for waste comprising radioactive Cs+ |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201310644030.1A CN103680660A (en) | 2013-12-03 | 2013-12-03 | Application of cullet in solidifying radionuclide and normal temperature solidifying method for waste comprising radioactive Cs+ |
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|---|---|
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ID=50317950
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|---|---|---|---|
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106328237A (en) * | 2015-06-29 | 2017-01-11 | 中国辐射防护研究院 | Radioactive spent ion exchange resin microwave carbonization and ashing process and special device |
| CN110291592A (en) * | 2017-01-06 | 2019-09-27 | 乔罗克国际股份有限公司 | Method for treatment fluid waste |
| CN111145931A (en) * | 2020-02-17 | 2020-05-12 | 南华大学 | Method for treating radioactive solid waste |
| CN112466503A (en) * | 2020-12-29 | 2021-03-09 | 西南科技大学 | Preparation method of glass ceramic body for solidifying Cs-containing soil |
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| CN111145931B (en) * | 2020-02-17 | 2020-09-08 | 南华大学 | Method for treating radioactive solid waste |
| CN112466503A (en) * | 2020-12-29 | 2021-03-09 | 西南科技大学 | Preparation method of glass ceramic body for solidifying Cs-containing soil |
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Application publication date: 20140326 |