CN108585722B - Cement-based curing material for curing waste liquid containing high-concentration boric acid nuclei and curing method thereof - Google Patents
Cement-based curing material for curing waste liquid containing high-concentration boric acid nuclei and curing method thereof Download PDFInfo
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- CN108585722B CN108585722B CN201810331576.4A CN201810331576A CN108585722B CN 108585722 B CN108585722 B CN 108585722B CN 201810331576 A CN201810331576 A CN 201810331576A CN 108585722 B CN108585722 B CN 108585722B
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- 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
- C04B28/12—Hydraulic lime
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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
- G21F9/165—Cement or cement-like matrix
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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
- G21F9/20—Disposal of liquid waste
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- 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
- C04B2111/00025—Aspects relating to the protection of the health, e.g. materials containing special additives to afford skin protection
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- 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
- C04B2201/00—Mortars, concrete or artificial stone characterised by specific physical values
- C04B2201/50—Mortars, concrete or artificial stone characterised by specific physical values for the mechanical strength
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- Inorganic Chemistry (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
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- Ceramic Engineering (AREA)
- Environmental & Geological Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Structural Engineering (AREA)
- Organic Chemistry (AREA)
- Processing Of Solid Wastes (AREA)
- Curing Cements, Concrete, And Artificial Stone (AREA)
Abstract
The invention relates to a cement-based curing material for curing high-concentration boric acid core waste liquid and a curing method thereof. The cement-based curing material comprises a cementing material, a modifier and an additive; the cementing material comprises cement, bentonite and lime; the modifier comprises magnesium-aluminum layered double hydroxide, lithium hydroxide and ammonium sulfate; the additive comprises welan gum and a naphthalene water reducer; in the cementing material, 75-85 wt% of cement, 5-10 wt% of lime and 10-15 wt% of bentonite are contained, and the sum of the cement, the lime and the bentonite is 100 wt%: the magnesium-aluminum layered double hydroxide accounts for 0.3-0.5% of the total mass of the cementing material, the lithium hydroxide accounts for 0.2-0.4% of the total mass of the cementing material, and the ammonium sulfate accounts for 0.5-0.8% of the total mass of the cementing material. Compared with the prior art, the cement-based curing material prepared by the invention has the advantages that the compressive strength value of the curing body 28d is as high as 24.7MPa, which is higher than 7MPa, the requirements of EJ 1186-.
Description
Technical Field
The invention relates to a curing material for treating radioactive nuclear waste, in particular to a cement-based curing material for curing high-concentration boric acid nuclear waste liquid and a curing method thereof.
Background
With the rapid development of the nuclear energy industry, the treatment and disposal of nuclear waste materials are receiving more and more attention from people. Nuclear waste is the nuclear ash left over after the combustion of nuclear substances in nuclear reactors (atomic furnaces), has extremely strong radioactivity, and has a half-life of thousands of years, tens of thousands of years or even hundreds of thousands of years. If the radioactive nuclear waste enters the environment, the radioactive nuclear waste can pollute the air, water and soil and further enter the human body through various ways. The ionizing radiation of the radioactive nuclear waste can act on the organism, cause damage to biological molecules, and cause metabolic disorder, functional and mechanical damage and even death of cells. Therefore, the world countries are actively seeking ways for the treatment of nuclear waste.
At present, alternative curing techniques are cement curing, glass curing, asphalt curing, plastic curing, artificial rock curing, and the like, depending on the form, nature, and purpose of treatment of the waste. The cement curing technology has the advantages of simple process, low requirement on equipment, no need of high temperature, easily available raw materials, high production capacity, stable hydration products, no problem of waste gas purification, low investment and operation cost, and small secondary pollution during curing production, is widely considered as an economic and effective curing method, and has been widely applied to the treatment of medium and low radioactive nuclear waste.
However, in the case of a nuclear waste liquid containing boric acid at a high concentration, boric acid forms a calcium borate coating layer on the surface of a hydration layer of cement particles, effectively inhibiting hydration, and delaying the setting of cement by delaying the formation of ettringite. When the boric acid concentration is too high, boric acid can inhibit the formation of ettringite. This results in insufficient early strength of the cured body, which in turn affects the development of later strength of the cured body, such that the strength value of the cured body 28d cannot meet engineering requirements. Therefore, the method removes the delayed coagulation of boric acid in the nuclear waste liquid on the cement-based material, and improves the compressive strength of the solidified body, thereby becoming a key technology for treating the nuclear waste containing high-concentration boric acid.
Disclosure of Invention
The invention aims to provide a cement-based curing material for curing high-concentration boric acid core waste liquid and a curing method thereof. The material can weaken the retarding effect of boric acid in the nuclear waste on the cement-based material, and simultaneously improve the compressive strength of a cement solidified body.
In order to achieve the purpose, the technical scheme disclosed by the invention is as follows:
a cement-based solidified material for solidifying waste liquid containing high-concentration boric acid nuclei comprises a gelled material, a modifier and an additive; the cementing material comprises cement, bentonite and lime; the modifier comprises magnesium-aluminum layered double hydroxide, lithium hydroxide and ammonium sulfate; the additive comprises welan gum and a naphthalene water reducer; in the cementing material, 75-85 wt% of cement, 5-10 wt% of lime and 10-15 wt% of bentonite are contained, and the sum of the cement, the lime and the bentonite is 100 wt%: the magnesium-aluminum layered double hydroxide accounts for 0.3-0.5% of the total mass of the cementing material, the lithium hydroxide accounts for 0.2-0.4% of the total mass of the cementing material, and the ammonium sulfate accounts for 0.5-0.8% of the total mass of the cementing material.
In the scheme, the welt gum accounts for 0.2-0.3% of the total mass of the cementing material, and the naphthalene water reducer accounts for 0.2-0.3% of the total mass of the cementing material.
In the above scheme, the volume weight of the cured material is: 1780kg/m 3-1920 kg/m 3.
In the scheme, the dosage of the nuclear waste liquid in each cubic meter of the cement-based curing material is 630 kg-710 kg.
In the above scheme, the high-concentration boric acid core waste liquid refers to boric acid with a mass concentration of more than 3%.
The cement and the lime are used as cementing materials to provide cementing capacity and strength; the bentonite has the function of adsorbing and solidifying radioactive elements in the nuclear waste liquid; the magnesium-aluminum layered double hydroxide, the lithium hydroxide and the ammonium sulfate are used as modifiers, the magnesium-aluminum layered double hydroxide has the effects of adsorbing radioactive elements in nuclear waste liquid and improving the durability of the cement-based material, the lithium hydroxide has the effect of promoting the condensation of the cement-based material, and the ammonium sulfate has the effect of prolonging the condensation time of the cement-based material; the functions of the welan gum and the naphthalene water reducing agent are to improve the workability of the cement-based curing material and improve the comprehensive performance of the cement cured body.
The curing method of the cement-based curing material comprises the following steps: fully mixing cement, bentonite, lime, magnesium-aluminum layered double hydroxide, lithium hydroxide, ammonium sulfate, welan gum and a naphthalene water reducer according to a preset proportion, then adding nuclear waste liquid into the mixture, and fully mixing and stirring.
The curing method of the cement-based curing material comprises the following steps: fully mixing cement, bentonite, lime, welan gum and a naphthalene water reducer according to a preset proportion to obtain powder, adding magnesium-aluminum layered double hydroxide, lithium hydroxide and ammonium sulfate into the nuclear waste liquid according to a preset proportion, fully stirring uniformly, and then mixing and stirring uniformly the powder and the nuclear waste liquid. In this method, the modifier is first mixed with the nuclear waste and then mixed with the premixed powder, which differs from the first method in that: magnesium-aluminum layered double hydroxide can preferentially adsorb and solidify radioactive elements in the nuclear waste liquid, and simultaneously, lithium hydroxide and ammonium sulfate can be mixed with borate in the nuclear waste liquid in advance, so that the modifier is uniformly distributed in the nuclear waste liquid, and after the modifier is mixed and stirred with powder, the removing effect on the retarding effect of the borate can be improved, thereby better exerting the synergistic effect of three components in the modifier and better improving the compressive strength of a cement solidified body.
The invention has the following beneficial effects: compared with the prior art, the cement-based curing material prepared by the invention has the compressive strength value of the curing body 28d as high as 24.7MPa which is higher than 7MPa, greatly meets the requirement of EJ 1186-.
Detailed Description
The present invention will be further illustrated by the following examples, but the present invention is not limited to the following examples, and the examples should not be construed as limiting the present invention.
Example 1
The embodiment provides a cement-based curing material for curing waste liquid containing high-concentration boric acid nuclei, which comprises the following components in percentage by weight:
PI 52.5 cement: 75 percent of
Bentonite: 15 percent of
Lime: 10 percent of
Magnesium-aluminum layered double hydroxide: 0.3 percent of the total amount of the cement, the bentonite and the lime
Lithium hydroxide: 0.2 percent of the total amount of the cement, the bentonite and the lime
Ammonium sulfate is 0.5 percent of the total amount of cement, bentonite and lime
Rubber for a warm wheel: 0.2 percent of the total amount of the cement, the bentonite and the lime
Naphthalene water reducing agent: 0.2 percent of the total amount of the cement, the bentonite and the lime
Nuclear waste liquid: 37.3 percent of the total amount of the cement, the bentonite and the lime.
The embodiment also provides a curing method of the cement-based curing material, which comprises the following steps:
a. weighing all the powder materials according to a proportion, and adding the powder materials into a stirrer to be uniformly mixed;
b. and adding the weighed nuclear waste liquid into the uniformly mixed powder, and uniformly mixing and stirring.
Example 2
The embodiment provides a cement-based curing material for curing waste liquid containing high-concentration boric acid nuclei, which comprises the following components in percentage by weight:
PI 52.5 cement: 80 percent of
Bentonite: 12.5 percent
Lime: 7.5 percent
Magnesium-aluminum layered double hydroxide: 0.4 percent of the total amount of the cement, the bentonite and the lime
Lithium hydroxide: 0.3 percent of the total amount of the cement, the bentonite and the lime
Ammonium sulfate is 0.65 percent of the total amount of cement, bentonite and lime
Rubber for a warm wheel: 0.25 percent of the total amount of the cement, the bentonite and the lime
Naphthalene water reducing agent: 0.25 percent of the total amount of the cement, the bentonite and the lime
Nuclear waste liquid: 37.3 percent of the total amount of the cement, the bentonite and the lime.
The embodiment also provides a curing method of the cement-based curing material, which comprises the following steps:
a. weighing the cementing material and the additive according to a ratio, and adding the materials into a stirrer to be uniformly mixed;
b. weighing the modifier according to a proportion, adding the modifier into the nuclear waste liquid, and uniformly mixing;
c. and mixing and stirring the powder and the nuclear waste liquid uniformly.
Example 3
The embodiment provides a cement-based curing material for curing waste liquid containing high-concentration boric acid nuclei, which comprises the following components in percentage by weight:
PI 52.5 cement: 85 percent of
Bentonite: 10 percent of
Lime: 5 percent of
Magnesium-aluminum layered double hydroxide: 0.5 percent of the total amount of the cement, the bentonite and the lime
Lithium hydroxide: 0.4 percent of the total amount of the cement, the bentonite and the lime
Ammonium sulfate is 0.8 percent of the total amount of cement, bentonite and lime
Rubber for a warm wheel: 0.3 percent of the total amount of the cement, the bentonite and the lime
Naphthalene water reducing agent: 0.3 percent of the total amount of the cement, the bentonite and the lime
Nuclear waste liquid: 37.3 percent of the total amount of the cement, the bentonite and the lime.
The embodiment also provides a curing method of the cement-based curing material, which comprises the following steps:
a. weighing the cementing material and the additive according to a ratio, and adding the materials into a stirrer to be uniformly mixed;
b. weighing the modifier according to a proportion, adding the modifier into the nuclear waste liquid, and uniformly mixing;
c. and mixing and stirring the powder and the nuclear waste liquid uniformly.
The results of the compressive strength value test of the cured body 28d of the above example are shown in Table 1 below.
TABLE 1 compressive strength values of the cured bodies according to the invention
| Test items | 28d compressive Strength (MPa) |
| Standard requirements | 7 |
| Example 1 | 19.6 |
| Example 2 | 21.3 |
| Example 3 | 24.7 |
To illustrate the synergistic effect of the three components of the modifier of the present invention, the present invention will now be further illustrated with reference to comparative examples, in which one of the three components of the modifier is not added in each of the following comparative examples.
Comparative example 1
The comparative example provides a cement-based curing material for curing a high-concentration boric acid core waste liquid, which comprises the following components in percentage by weight:
PI 52.5 cement: 75 percent of
Bentonite: 15 percent of
Lime: 10 percent of
Magnesium-aluminum layered double hydroxide: is free of
Lithium hydroxide: 0.2 percent of the total amount of the cement, the bentonite and the lime
Ammonium sulfate is 0.5 percent of the total amount of cement, bentonite and lime
Rubber for a warm wheel: 0.2 percent of the total amount of the cement, the bentonite and the lime
Naphthalene water reducing agent: 0.2 percent of the total amount of the cement, the bentonite and the lime
Nuclear waste liquid: 37.3 percent of the total amount of the cement, the bentonite and the lime.
The comparative example also provides a method of curing the cement-based curing material, comprising the steps of:
a. weighing all the powder materials according to a proportion, and adding the powder materials into a stirrer to be uniformly mixed;
b. and adding the weighed nuclear waste liquid into the uniformly mixed powder, and uniformly mixing and stirring.
Comparative example 2
The comparative example provides a cement-based curing material for curing a high-concentration boric acid core waste liquid, which comprises the following components in percentage by weight:
PI 52.5 cement: 80 percent of
Bentonite: 12.5 percent
Lime: 7.5 percent
Magnesium-aluminum layered double hydroxide: 0.4 percent of the total amount of the cement, the bentonite and the lime
Lithium hydroxide: is free of
Ammonium sulfate is 0.65 percent of the total amount of cement, bentonite and lime
Rubber for a warm wheel: 0.25 percent of the total amount of the cement, the bentonite and the lime
Naphthalene water reducing agent: 0.25 percent of the total amount of the cement, the bentonite and the lime
Nuclear waste liquid: 37.3 percent of the total amount of the cement, the bentonite and the lime.
The comparative example also provides a method of curing the cement-based curing material, comprising the steps of:
a. weighing the cementing material and the additive according to a ratio, and adding the materials into a stirrer to be uniformly mixed;
b. weighing the modifier according to a proportion, adding the modifier into the nuclear waste liquid, and uniformly mixing;
c. and mixing and stirring the powder and the nuclear waste liquid uniformly.
Comparative example 3
The comparative example provides a cement-based curing material for curing a high-concentration boric acid core waste liquid, which comprises the following components in percentage by weight:
PI 52.5 cement: 85 percent of
Bentonite: 10 percent of
Lime: 5 percent of
Magnesium-aluminum layered double hydroxide: 0.5 percent of the total amount of the cement, the bentonite and the lime
Lithium hydroxide: 0.4 percent of the total amount of the cement, the bentonite and the lime
Ammonium sulfate of
Rubber for a warm wheel: 0.3 percent of the total amount of the cement, the bentonite and the lime
Naphthalene water reducing agent: 0.3 percent of the total amount of the cement, the bentonite and the lime
Nuclear waste liquid: 37.3 percent of the total amount of the cement, the bentonite and the lime.
The comparative example also provides a method of curing the cement-based curing material, comprising the steps of:
a. weighing the cementing material and the additive according to a ratio, and adding the materials into a stirrer to be uniformly mixed;
b. weighing the modifier according to a proportion, adding the modifier into the nuclear waste liquid, and uniformly mixing;
c. and mixing and stirring the powder and the nuclear waste liquid uniformly.
The results of the compressive strength value test of the comparative example cured body 28d are shown in Table 2 below.
TABLE 2 compressive strength values of comparative example cured bodies
| Comparative example | 28d compressive Strength (MPa) |
| Comparative example 1 | 9.4 |
| Comparative example 2 | 8.3 |
| Comparative example 3 | 10.6 |
While embodiments of the present invention have been described, the present invention is not limited to the above-described embodiments, which are intended to be illustrative rather than limiting, and many modifications may be made by those skilled in the art without departing from the spirit and scope of the invention as defined by the appended claims.
Claims (7)
1. The cement-based curing material for curing the waste liquid containing the high-concentration boric acid nuclei is characterized by comprising a cementing material, a modifier and an additive; the cementing material comprises cement, bentonite and lime; the modifier comprises magnesium-aluminum layered double hydroxide, lithium hydroxide and ammonium sulfate; the additive comprises welan gum and a naphthalene water reducer; in the cementing material, 75-85 wt% of cement, 5-10 wt% of lime and 10-15 wt% of bentonite are contained, and the sum of the cement, the lime and the bentonite is 100 wt%: the magnesium-aluminum layered double hydroxide accounts for 0.3-0.5% of the total mass of the cementing material, the lithium hydroxide accounts for 0.2-0.4% of the total mass of the cementing material, and the ammonium sulfate accounts for 0.5-0.8% of the total mass of the cementing material.
2. The cement-based solidifying material of claim 1, wherein the welt gum accounts for 0.2-0.3% of the total mass of the cementing material, and the naphthalene water reducing agent accounts for 0.2-0.3% of the total mass of the cementing material.
3. The cement-based cured material of claim 1, wherein the cured material has a bulk density of 1780kg/m3～1920kg/m3。
4. The cement-based cured material according to claim 1, wherein the amount of the nuclear waste liquid is 630kg to 710kg per cubic meter of the cement-based cured material.
5. The cement-based cured material according to claim 1, wherein the high-concentration boric acid nuclear waste liquid is boric acid having a mass concentration of more than 3%.
6. A method of curing a cementitious curing material as claimed in any one of claims 1 to 5, characterised in that the method is: fully mixing cement, bentonite, lime, magnesium-aluminum layered double hydroxide, lithium hydroxide, ammonium sulfate, welan gum and a naphthalene water reducer according to a preset proportion, then adding nuclear waste liquid into the mixture, and fully mixing and stirring.
7. A method of curing a cementitious curing material as claimed in any one of claims 1 to 5, characterised in that the method is: fully mixing cement, bentonite, lime, welan gum and a naphthalene water reducer according to a preset proportion to obtain powder, adding magnesium-aluminum layered double hydroxide, lithium hydroxide and ammonium sulfate into the nuclear waste liquid according to a preset proportion, fully stirring uniformly, and then mixing and stirring uniformly the powder and the nuclear waste liquid.
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| CN110330297B (en) * | 2019-06-26 | 2021-11-09 | 武汉理工大学 | Sulphoaluminate cement-based curing material for curing low-level waste liquid in high-concentration boric acid and curing method thereof |
| CN110342866B (en) * | 2019-07-30 | 2021-11-05 | 上海市建筑科学研究院 | Nuclear power station radioactive raffinate cement solidified body and preparation method thereof |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001097757A (en) * | 1999-09-30 | 2001-04-10 | Mitsubishi Heavy Ind Ltd | Cement hardener for boric acid, method for hardening cement for boric acid and cement hardened product |
| CN101337785A (en) * | 2008-08-06 | 2009-01-07 | 西南科技大学 | Sustained-release water reducing agent for cement concrete and method for preparing same |
| CN102208225A (en) * | 2011-05-19 | 2011-10-05 | 清华大学 | Method for solidifying radioactive boron-containing residual distillate by Portland cement |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001097757A (en) * | 1999-09-30 | 2001-04-10 | Mitsubishi Heavy Ind Ltd | Cement hardener for boric acid, method for hardening cement for boric acid and cement hardened product |
| CN101337785A (en) * | 2008-08-06 | 2009-01-07 | 西南科技大学 | Sustained-release water reducing agent for cement concrete and method for preparing same |
| CN102208225A (en) * | 2011-05-19 | 2011-10-05 | 清华大学 | Method for solidifying radioactive boron-containing residual distillate by Portland cement |
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