CN111524632A - Magnesium-based cement curing substrate and method for treating low-medium radioactive nuclear waste - Google Patents
Magnesium-based cement curing substrate and method for treating low-medium radioactive nuclear waste Download PDFInfo
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- CN111524632A CN111524632A CN202010348547.6A CN202010348547A CN111524632A CN 111524632 A CN111524632 A CN 111524632A CN 202010348547 A CN202010348547 A CN 202010348547A CN 111524632 A CN111524632 A CN 111524632A
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- magnesium
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- based cement
- curing
- waste
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Classifications
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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
- G21F9/28—Treating solids
- G21F9/34—Disposal of solid waste
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B28/00—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements
- C04B28/02—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements containing hydraulic cements other than calcium sulfates
- C04B28/10—Lime cements or magnesium oxide cements
- C04B28/105—Magnesium oxide or magnesium carbonate cements
-
- 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
- G21F9/165—Cement or cement-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
- G21F9/04—Treating liquids
- G21F9/20—Disposal of liquid waste
-
- 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
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2111/00—Mortars, concrete or artificial stone or mixtures to prepare them, characterised by specific function, property or use
- C04B2111/00474—Uses not provided for elsewhere in C04B2111/00
- C04B2111/00767—Uses not provided for elsewhere in C04B2111/00 for waste stabilisation purposes
- C04B2111/00775—Uses not provided for elsewhere in C04B2111/00 for waste stabilisation purposes the composition being used as waste barriers or the like, e.g. compositions used for waste disposal purposes only, but not containing the waste itself
Abstract
The invention relates to a magnesium-based cement curing base material for treating low-medium radioactive nuclear waste and a method thereof. The cement solidified body prepared by the system has good mechanical property, leaching resistance, freeze fusion resistance and soaking resistance, all indexes meet the national standard requirements, especiallyTwo nuclides with the greatest harm in low-level radioactive nuclear waste137Cs、90Sr shows excellent leaching resistance, and the leaching rate of 42d nuclear species ions is as low as 10‑4～5cm/d, the invention provides a novel cement-based curing material for the treatment and disposal of medium-low radioactive nuclear waste, and has wide application prospect.
Description
Technical Field
The invention relates to the technical field of nuclear waste treatment methods, in particular to a magnesium-based cement curing substrate and a method for treating low-medium radioactive nuclear waste.
Background
In China, since the first nuclear power station, Zhejiang sea salt Qinshan nuclear power station, in 1991 and grid-connected power generation, the China nuclear power industry develops rapidly and accounts for the total power generation amount in ChinaBy 4%, the size of the transport and installation machine reaches the third level of the world, and the size of the construction machine reaches the first level of the world. As a clean energy source, nuclear energy will play an increasingly important role in the energy system. However, in the process of developing and utilizing nuclear energy, the problems caused by the nuclear waste with large quantity are not ignored. Investigations have shown that nuclear waste with high radioactivity accounts for only about 1%, the remaining 99% are mainly low and medium radioactive nuclear waste, and cesium and strontium are two nuclides with the greatest harm, namely fission nuclides generated during the operation of a nuclear reactor, and have a longer half-life period (137The half-life of Cs is 30.2 years,90sr half-life 28.8 years), the specific gravity of radioactivity accounting for the total radioactivity of the mixed fission product is large, the mixed fission product exists in the form of ions, the mixed fission product is easy to migrate in water environment, and the enrichment effect can cause the canceration of organism cells to generate irreversible influence. Therefore, proper disposal of low-to-medium level waste, especially cesium and strontium, presents a significant challenge to the development of the nuclear power industry.
At present, the internationally generally accepted treatment mode of the medium-low nuclear waste is solidification treatment, wherein the waste is converted into solid, namely solidified body, by using materials such as ceramics, asphalt, cement and the like, the solidified body is packaged into a specified closed container, and the sealed body is sent to the underground for burying and storing through an automatic transportation system, so that the aim of permanently isolating the biosphere is achieved. The cement solidification is the earliest and most mature solidification method, has the advantages of simple equipment process, low cost and the like, but the wide application also exposes the defects of the traditional cement-based solidification material, and the coagulation and hardening of a common portland cement system are abnormal due to a large amount of salt introduced when the nuclide leaching rate is high, the tolerance is small, and the waste treatment capacity is too large. Therefore, the development of a novel cement-based curing material can improve the leaching resistance of curing and the stability of a system, and has great significance for the safe treatment of nuclear waste.
Disclosure of Invention
The invention aims to solve the technical problem of overcoming the defects of the prior art and provide a magnesium-based cement curing material for treating medium-low radioactive nuclear wastes and a preparation method thereof, wherein the magnesium-based cement curing material has stable comprehensive performance and low leaching rate of nuclide ions.
In order to solve the technical problems, the technical scheme provided by the invention is as follows: the magnesium-based cement curing material for treating medium and low radioactive nuclear wastes comprises, by mass ratio, 20-40% of light-burned magnesium oxide, 30-60% of silica fume, 1-2% of sodium salt/potassium salt additive and 0-3% of nitrate/chloride salt, and the water-cement ratio of the system is established according to a water consumption experiment of standard consistency.
A method for treating a magnesium-based cement-cured substrate of low to medium radioactive nuclear waste, said method comprising the following operative steps:
the method comprises the following steps: weighing main raw materials of the curing substrate, light-burned magnesium oxide and a high-activity silicon source powder material, weighing, mechanically mixing for 10-20 min, and keeping drying to obtain mixed powder;
step two: dissolving the admixture in water, adding the dissolved admixture, the radioactive waste material and the quartz sand into the mixed powder in the step one, and stirring the mixture into slurry with good working performance by using a cement mortar stirrer;
step three: and (3) putting the slurry obtained in the step two into a mold, putting the mold into a constant temperature and humidity box, curing for 1-2 d, then removing the mold, and continuously curing the cured body to the specified age, wherein the curing condition is that the temperature is 25 +/-2 ℃ and the humidity is more than or equal to 95%.
Further, the light-burned magnesia MgO in the step one is prepared from magnesite MgCO3Calcining at 750-800 deg.C to obtain the product, wherein the MgO content is above 90%, and the particle size of the powder is 10 μm.
Further, the high-activity silicon source in the step one is prepared from the homogeneous material of granulated blast furnace slag, fly ash or silica fume, SiO2The content of (B) is more than 95%, and the particle size is usually 100-300 nm.
Furthermore, the additive in the second step is a sodium salt/potassium salt, so that the working performance of the system can be improved.
Furthermore, the quartz sand added in the second step is used for improving the dry shrinkage defect of the system, the particle size distribution range is 5-500 μm, and D50 is 168.84 μm.
Further, the cured body prepared by stirring in the third step is taken into consideration of experimental safetyThe nuclear waste provides non-radioactive nuclide ions Cs by using chlorine salt and nitrate analysis pure reagents+、Sr2+Substitution of two most harmful representative nuclides in nuclear waste137Cs、90Sr。
Firstly, weighing a plurality of parts of the components according to the mass ratio for later use, and uniformly mixing light-burned magnesium oxide and silica fume powder by using a stirrer for 10-20 min; secondly, preparing a modified additive aqueous solution; then adding the uniformly mixed magnesium oxide and silica fume powder into the aqueous solution for 2-3 times, and stirring the mixture into slurry with good fluidity by using a cement stirrer at an accelerated speed; and finally, filling the stirred slurry into a mold, putting the mold into a constant temperature and humidity box, curing for 1d, then removing the mold, and continuing curing to a specified age for performance test, wherein the curing conditions are as follows: the temperature is 25 +/-2 ℃, and the humidity is more than or equal to 95 percent.
The invention relates to a low radioactive nuclear waste solidified material in magnesium-based cement, which utilizes light-burned MgO and active SiO2Reacting at normal temperature to finally generate a hydrated magnesium silicate gel system (MgO-SiO) of hydrated magnesium silicate gel (M-S-H)2-H2O). The pore solution environment of the system has a low pH value, and hardly reacts with aluminum-containing waste to generate H2The nuclear waste containing active metals such as aluminum and the like can be effectively packaged. In addition, the hydrated magnesium silicate gel system has a porous structure and a specific surface area of 200m2/g-1And the composite material has excellent adsorption performance, and can exert great advantages in the aspect of curing treatment of nuclear waste.
The invention has the beneficial effects that: the magnesium-based cement curing base material for treating the low-medium radioactive nuclear waste has excellent leaching resistance. The detection of relevant indexes of the solidified body made of the solidified base material is carried out according to the requirements of the national standard specification ' Standard leaching experiment method of Low and Medium horizontal radioactive waste solidified body ' (GB/T7023-2011) and the performance requirement of Low and Medium horizontal radioactive waste solidified body, namely the cement solidified body ' (GB 14569.1-2011), and the result shows that the compressive strength of the magnesium-based cement solidified body cured for 28d under the standard curing condition is between 23 and 36MPa (the standard: the compressive strength of 28d is over 7 MPa); when the leaching solution is deionized waterThe 42d leaching rate of the solidified body to the nuclide Cs is 6.4 × 10-5The cumulative leaching rate of cm/d and 42d is about 0.01cm, and the leaching rate of 42d of the nuclide Sr is 4.6 × 10-4The accumulated leaching fractions of cm/d and 42d are about 0.07cm and are far lower than the standard limit value required by the specification; meanwhile, the solidified body also has good impact resistance, soaking resistance and freeze-thaw resistance, meets the national standard requirements which the cement solidified body should meet, and has wide application prospect in the treatment of nuclear waste.
Detailed Description
The present invention will be described in further detail with reference to examples.
Example 1
Weighing the nuclein used for treating the low-and-medium-grade radioactive nuclear waste according to the following proportion137Cs magnesium-based cement setting raw material: (unit: g)
TABLE 1. containing137Sample proportion of Cs magnesium-based cement solidified body
| Numbering | Light-burned magnesium | Silica fume | Quartz sand | Sodium salt additive | Cesium chloride | Water (W) |
| A1 | 300 | 450 | 750 | 15 | 3.8 | 487.5 |
| A2 | 300 | 450 | 750 | 15 | 7.6 | 487.5 |
| A3 | 300 | 450 | 750 | 15 | 15 | 487.5 |
Mixing the weighed light-burned magnesium and silica fume, and stirring uniformly for 15 min; adding the mixed powder and cesium chloride into the additive aqueous solution for 2-3 times, accelerating into slurry by using a cement mortar stirrer, putting the slurry into a mold, and putting the mold into a standard curing box for curing for 1d for demolding; and continuously placing the formed solidified body into a standard curing box for curing to 28d and 42 d.
According to the national standard specification 'Standard Leaching Experimental method for Low and Medium horizontal radioactive waste solidified bodies' (GB/T7023-2011) and 'Performance requirement of Low and Medium horizontal radioactive waste solidified bodies' (GB 14569.1-2011), relevant index tests are carried out on the magnesium-based cement solidified bodies which are cured to corresponding ages and taken out, wherein the relevant index tests comprise the compressive strength, leaching resistance, impact resistance, soaking resistance and freeze-thaw resistance of the solidified bodies. The test results are shown in table 2 below:
TABLE 2. containing137Various performance test results of Cs magnesium-based cement solidified body
From the test results in table 2, the magnesium-based cement solidified body can meet the requirements of national standard specifications on various performance indexes of the cement solidified body, one of the most harmful nuclides in the medium-low nuclear waste,137and the Cs has excellent leaching resistance, and the compressive strength is increased after the Cs is soaked in water for 90 days, so that the Cs shows good leaching resistance, and the safety and the stability of a solidified body in an accidental contact water environment can be ensured.
Example 2
Weighing the nuclein used for treating the low-and-medium-grade radioactive nuclear waste according to the following proportion90Magnesium-based cement curing raw material of Sr: (unit: g)
TABLE 3. containing90Sample proportion of Sr magnesium-based cement solidified body
| Numbering | Light-burned magnesium | Silica fume | Quartz sand | Sodium salt additive | Strontium nitrate | Water (W) |
| B1 | 300 | 450 | 750 | 15 | 14.5 | 525 |
| B2 | 300 | 450 | 750 | 15 | 29.0 | 525 |
| B3 | 300 | 450 | 750 | 15 | 57.9 | 525 |
Mixing the weighed light-burned magnesium and silica fume, and stirring uniformly for 15 min; adding the mixed powder and strontium nitrate into the additive aqueous solution for 2-3 times, accelerating into slurry by using a cement mortar stirrer, putting the slurry into a mold, and putting the mold into a standard curing box for curing for 1d for demolding; and continuously placing the formed solidified body into a standard curing box for curing to 28d and 42 d.
According to the national standard specification ' Standard leaching experiment method of low and medium horizontal radioactive waste solidified bodies ' (GB/T7023-2011) and ' performance requirements of low and medium horizontal radioactive waste solidified bodies ' -cement solidified bodies ' (GB 14569.1-2011), the magnesium-based cement solidified bodies cured to corresponding ages are taken out for testing, and the test comprises the compression strength, leaching resistance, impact resistance, soaking resistance and freeze-thaw resistance of the solidified bodies. The test results are shown in table 4 below:
TABLE 4. containing90Various performance test results of Sr magnesium-based cement solidified body
As can be seen from the performance test results in Table 4, the magnesium-based cement material provided by the present invention was used to prepare cement materials containing magnesium90The Sr solidified body is feasible, and all performance indexes of the solidified body meet the requirements of national standard specifications on cement solidified bodies.
The mechanical properties and various durability properties of the cement solidified body prepared by the magnesium-based cement solidified base material and the using method provided by the invention are illustrated through the specific examples. In general, the mechanical property of the magnesium-based cement solidified body is stable, the compressive strength of the solidified body maintained for 28 days in a standard environment can reach about 25MPa, good integrity can be still kept after an impact resistance test is carried out, and the accidental leakage risk of nuclide ions in the solidified body transportation process is greatly reduced; for two nuclides with the greatest harm in medium-low radioactive nuclear waste137Cs、90Sr, the magnesium-based cement solidified body also shows good leaching resistance, and the leaching rate of 42d nuclide ions can be as low as 10-4～5cm/d, far exceeding the limit value required in the national standard specification; the good freeze-thaw resistance and soaking resistance of the solidified body also ensure the safety of long-term underground burying. In addition, the preparation process of the curing base material is simple and pollution-free, and from the aspect of environmental protection, no matter the curing base material is used for building material products or medium-low level waste, the magnesium-based cement system provided by the invention has great development and utilization potential, and has very important significance for magnesium resource development and environmental protection in China.
Although the invention has been described in detail hereinabove with respect to a general description and specific embodiments thereof, it will be apparent to those skilled in the art that modifications or improvements may be made thereto based on the invention. Accordingly, such modifications and improvements are intended to be within the scope of the invention as claimed.
Claims (7)
1. A method for treating magnesium-based cement-cured substrates of low-to-medium radionuclide waste, characterized in that it comprises the following operative steps:
the method comprises the following steps: weighing main raw materials of the curing substrate, light-burned magnesium oxide and a high-activity silicon source powder material, weighing, mechanically mixing for 10-20 min, and keeping drying to obtain mixed powder;
step two: dissolving the admixture in water, adding the dissolved admixture, the radioactive waste material and the quartz sand into the mixed powder in the step one, and stirring the mixture into slurry with good working performance by using a cement mortar stirrer;
step three: and (3) putting the slurry obtained in the step two into a mold, putting the mold into a constant temperature and humidity box, curing for 1-2 d, then removing the mold, and continuously curing the cured body to the specified age, wherein the curing condition is that the temperature is 25 +/-2 ℃ and the humidity is more than or equal to 95%.
2. A method of treating a low radionuclide waste magnesium based cement cured substrate according to claim 1 characterized by: the light-burned magnesia MgO in the step one is prepared from magnesite MgCO3Calcining at 750-800 deg.C to obtain the product, wherein the MgO content is above 90%, and the particle size of the powder is 10 μm.
3. A method of treating a low radionuclide waste magnesium based cement cured substrate according to claim 1 characterized by: the high-activity silicon source in the step one is prepared from homogeneous materials of granulated blast furnace slag, fly ash or silica fume, SiO2The content of (B) is more than 95%, and the particle size is usually 100-300 nm.
4. A method of treating a low radionuclide waste magnesium based cement cured substrate according to claim 1 characterized by: and the additive in the second step is a sodium salt/potassium salt, so that the working performance of the system can be improved.
5. A method of treating a low radionuclide waste magnesium based cement cured substrate according to claim 1 characterized by: the quartz sand added in the second step is used for improving the dry shrinkage defect of the system, the particle size distribution range is 5-500 mu m, and D50 is 168.84 mu m.
6. A method of treating a low radionuclide waste magnesium based cement cured substrate according to claim 1 characterized by: based on the consideration of experimental safety, the nuclear waste required by the stirred solidified body in the third step is provided with non-radioactive nuclide ions Cs by chlorine salt and nitrate analytical pure reagent+、Sr2+Substitution of two most harmful representative nuclides in nuclear waste137Cs、90Sr。
7. A magnesium based cement cured substrate obtainable by any one of claims 1 to 5, wherein: the magnesium-based cement curing base material comprises the following components in percentage by mass: 20-40% of light-burned magnesia, 30-60% of silica fume, 1-2% of an additive and 0-3% of nitrate or chloride, and the water-cement ratio of the system is determined according to the water consumption of standard consistency.
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| CN202010348547.6A CN111524632A (en) | 2020-04-28 | 2020-04-28 | Magnesium-based cement curing substrate and method for treating low-medium radioactive nuclear waste |
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| CN202010348547.6A CN111524632A (en) | 2020-04-28 | 2020-04-28 | Magnesium-based cement curing substrate and method for treating low-medium radioactive nuclear waste |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114719268A (en) * | 2022-03-15 | 2022-07-08 | 中核四川环保工程有限责任公司 | Method for solidifying incineration pyrolysis ash of low-emission organic waste liquid |
| CN115490500A (en) * | 2022-09-20 | 2022-12-20 | 大连理工大学 | Formula and preparation method of magnesium cement solidified radioactive waste resin |
-
2020
- 2020-04-28 CN CN202010348547.6A patent/CN111524632A/en not_active Withdrawn
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114719268A (en) * | 2022-03-15 | 2022-07-08 | 中核四川环保工程有限责任公司 | Method for solidifying incineration pyrolysis ash of low-emission organic waste liquid |
| CN115490500A (en) * | 2022-09-20 | 2022-12-20 | 大连理工大学 | Formula and preparation method of magnesium cement solidified radioactive waste resin |
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