CN117658462A - Starting glass for joule heating ceramic electric melting furnace suitable for solidifying power stack high-level waste liquid glass, and preparation and application thereof - Google Patents

Starting glass for joule heating ceramic electric melting furnace suitable for solidifying power stack high-level waste liquid glass, and preparation and application thereof Download PDF

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Publication number
CN117658462A
CN117658462A CN202311650282.5A CN202311650282A CN117658462A CN 117658462 A CN117658462 A CN 117658462A CN 202311650282 A CN202311650282 A CN 202311650282A CN 117658462 A CN117658462 A CN 117658462A
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China
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glass
waste liquid
power stack
level waste
melting furnace
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CN202311650282.5A
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Chinese (zh)
Inventor
朱永昌
杨德博
崔竹
焦云杰
齐建平
董炫疆
岳汉威
赵永祥
赵鲲
郭建峰
杜瞻远
王东宇
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China Building Materials Academy CBMA
China National Building Material Group Co Ltd CNBM
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China Building Materials Academy CBMA
China National Building Material Group Co Ltd CNBM
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Priority to CN202311650282.5A priority Critical patent/CN117658462A/en
Publication of CN117658462A publication Critical patent/CN117658462A/en
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    • CCHEMISTRY; METALLURGY
    • C03GLASS; MINERAL OR SLAG WOOL
    • C03CCHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C3/00Glass compositions
    • C03C3/04Glass compositions containing silica
    • C03C3/076Glass compositions containing silica with 40% to 90% silica, by weight
    • C03C3/095Glass compositions containing silica with 40% to 90% silica, by weight containing rare earths
    • CCHEMISTRY; METALLURGY
    • C03GLASS; MINERAL OR SLAG WOOL
    • C03BMANUFACTURE, SHAPING, OR SUPPLEMENTARY PROCESSES
    • C03B5/00Melting in furnaces; Furnaces so far as specially adapted for glass manufacture
    • C03B5/16Special features of the melting process; Auxiliary means specially adapted for glass-melting furnaces
    • CCHEMISTRY; METALLURGY
    • C03GLASS; MINERAL OR SLAG WOOL
    • C03CCHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C3/00Glass compositions
    • C03C3/04Glass compositions containing silica
    • C03C3/062Glass compositions containing silica with less than 40% silica by weight
    • C03C3/064Glass compositions containing silica with less than 40% silica by weight containing boron
    • C03C3/068Glass compositions containing silica with less than 40% silica by weight containing boron containing rare earths
    • GPHYSICS
    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21FPROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/04Treating liquids
    • G21F9/06Processing
    • G21F9/16Processing by fixation in stable solid media
    • G21F9/162Processing by fixation in stable solid media in an inorganic matrix, e.g. clays, zeolites

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Geochemistry & Mineralogy (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Inorganic Chemistry (AREA)
  • Glass Compositions (AREA)

Abstract

The invention belongs to the technical field of high-level waste liquid treatment, and provides starting glass for a joule heating ceramic electric melting furnace for solidifying power stack high-level waste liquid glass, and preparation and application thereof. The starting glass comprises the following components in percentage by mass: siO (SiO) 2 35~55%,B 2 O 3 9~15%,Na 2 O 6~14%,Li 2 O 1~3%,Al 2 O 3 3~6%,CaO 5~8.3%,MgO 0.3~2.08%,BaO 1.03~3.13%,V 2 O 5 0.2~2.3%,Sb 2 O 5 0.3~2%,ZrO 2 1~3%,La 2 O 3 3~6%,CeO 2 0.3~1.8%,MoO 3 1 to 2.8 percent. The starting glass provided by the invention ensures the safety of starting and replacing the joule heating ceramic electric melting furnace in the power stack high-level waste liquid glass curing process.

Description

Starting glass for joule heating ceramic electric melting furnace suitable for solidifying power stack high-level waste liquid glass, and preparation and application thereof
Technical Field
The invention relates to the technical field of high-level waste liquid treatment, in particular to starting glass for a joule heating ceramic electric melting furnace for solidifying power stack high-level waste liquid glass, and preparation and application thereof.
Background
The spent fuel used in the nuclear power station is a mixture with very complex components from the chemical point of view, mainly comprises four components such as uranium oxide, (oxidized) plutonium, fission Products (FP) and minor actinides, and has the characteristics of complex components, more than 40 elements, more than 100 isotopes, strong radioactivity, high biotoxicity, long half-life and the like.
In particular to the power stack high-level discharge waste liquid which contains forty kinds of components, mainly contains alkali metal, lanthanoid and fission elements (No. 30-70 elements), wherein Al 2 O 3 The content is 5-20wt%; the total content of the yellow phase element sulfur, molybdenum and the like is higherLow, less than 2wt%; the total content of noble metals Ru, rh, pd, etc. is less than 3wt%.
The method is characterized in that the high-level waste liquid is treated in the internationally existing commercial spent fuel post-treatment plant in a glass solidification mode, and the glass solidification process is to mix the high-level waste liquid with glass materials according to a certain proportion, and then obtain stable glass or glass-like solid after the high-level waste liquid is melted at a high temperature (900-1200 ℃) by using a Joule heating ceramic electric melting furnace.
When glass solidification is performed by using a joule-heated ceramic electric melting furnace, the joule-heated ceramic electric melting furnace needs to be started and cleaned by using starting glass. The prior art does not relate to starting glass for solidifying high level waste liquid by utilizing a joule heating ceramic electric melting furnace for power.
Disclosure of Invention
In view of the above, the present invention aims to provide a starting glass for a joule heating ceramic electric melting furnace suitable for solidifying power stack high level waste liquid glass, and preparation and application thereof. The starting glass provided by the invention can be used for starting and cleaning the joule heating ceramic electric melting furnace for solidifying the power stack high-level waste liquid glass.
In order to achieve the above object, the present invention provides the following technical solutions:
the invention provides a starting glass for a joule heating ceramic electric melting furnace for solidifying power stack high-level waste liquid glass, which comprises the following components in percentage by mass:
SiO 2 35~55%,B 2 O 3 9~15%,Na 2 O 6~14%,Li 2 O 1~3%,Al 2 O 3 3~6%,CaO 5~8.3%,MgO 0.3~2.08%,BaO 1.03~3.13%,V 2 O 5 0.2~2.3%,Sb 2 O 5 0.3~2%,ZrO 2 1~3%,La 2 O 3 3~6%,CeO 2 0.3~1.8%,MoO 3 1~2.8%。
the invention also provides a preparation method of the starting glass for the joule heating ceramic electric melting furnace, which is suitable for curing the power stack high-level waste liquid glass and comprises the following steps of:
grinding and mixing the components to obtain mixed powder;
and (3) sequentially melting and pouring the mixed powder to obtain the starting glass for the joule heating ceramic electric melting furnace, which is suitable for solidifying the power stack high-level waste liquid glass.
Preferably, the melting temperature is 1150-1300 ℃ and the melting time is 3-5 h.
The invention also provides the application of the starting glass for the joule heating ceramic electric melting furnace for curing the power stack high-level waste liquid glass or the starting glass for the joule heating ceramic electric melting furnace for curing the power stack high-level waste liquid glass, which is obtained by the preparation method of the technical scheme, in the treatment of the power stack high-level waste liquid.
The invention provides a starting glass for a joule heating ceramic electric melting furnace for solidifying power stack high-level waste liquid glass, which comprises the following components in percentage by mass: siO (SiO) 2 35~55%,B 2 O 3 9~15%,Na 2 O 6~14%,Li 2 O 1~3%,Al 2 O 3 3~6%,CaO 5~8.3%,MgO 0.3~2.08%,BaO1.03~3.13%,V 2 O 5 0.2~2.3%,Sb 2 O 5 0.3~2%,ZrO 2 1~3%,La 2 O 3 3~6%,CeO 2 0.3~1.8%,MoO 3 1 to 2.8 percent. The starting glass provided by the invention ensures that the operation basic performance of the electric melting furnace of the joule heating ceramic, such as the electric performance and the viscosity performance, can meet the operation requirement of the electric melting furnace of the joule heating ceramic; on the other hand, the component design in the replacement process does not influence the fact that the component fluctuation of the final product in the curing treatment process in the joule heating ceramic electric melting furnace is not large, namely the component change of the starting glass and the glass curing body product containing the power stack high-level waste liquid is not large. Therefore, the starting glass provided by the invention ensures the safety of starting and replacing the joule heating ceramic electric melting furnace in the process of solidifying the power stack high-level waste liquid glass.
Detailed Description
The invention provides a starting glass for a joule heating ceramic electric melting furnace for solidifying power stack high-level waste liquid glass, which comprises the following components in percentage by mass:
SiO 2 35~55%,B 2 O 3 9~15%,Na 2 O 6~14%,Li 2 O 1~3%,Al 2 O 3 3~6%,CaO 5~8.3%,MgO 0.3~2.08%,BaO 1.03~3.13%,V 2 O 5 0.2~2.3%,Sb 2 O 5 0.3~2%,ZrO 2 1~3%,La 2 O 3 3~6%,CeO 2 0.3~1.8%,MoO 3 1~2.8%。
in the present invention, the raw materials used in the present invention are preferably commercially available products unless otherwise specified.
The starting glass for the joule heating ceramic electric melting furnace suitable for solidifying the power stack high-level waste liquid glass comprises 35-55% of SiO by mass percent 2 Preferably 40 to 52%, more preferably 45 to 50%.
The starting glass for the joule heating ceramic electric melting furnace suitable for solidifying the power stack high-level waste liquid glass provided by the invention comprises 9-15% by mass of B 2 O 3 Preferably 10 to 14%, more preferably 11 to 13%.
The starting glass for the joule heating ceramic electric melting furnace suitable for solidifying the power stack high-level waste liquid glass comprises 6-14% of Na by mass 2 O is preferably 8 to 12%.
The starting glass for the joule heating ceramic electric melting furnace suitable for solidifying the power stack high-level waste liquid glass provided by the invention comprises 1-3% of Li by mass percent 2 O is preferably 1.47 to 2.52%.
The starting glass for the joule heating ceramic electric melting furnace suitable for solidifying the power stack high-level waste liquid glass provided by the invention comprises 3-6% of Al by mass percent 2 O 3 Preferably 4 to 5.5%.
The starting glass for the joule heating ceramic electric melting furnace suitable for solidifying the power stack high-level waste liquid glass provided by the invention comprises 5-8.3% of CaO, preferably 6-8% of CaO, and more preferably 6.5-7.5% of CaO.
The starting glass for the joule heating ceramic electric melting furnace, which is suitable for solidifying the power stack high-level waste liquid glass, comprises MgO with the mass percent of 0.3-2.08%, preferably 1-2%.
The starting glass for the joule heating ceramic electric melting furnace, which is suitable for solidifying the power stack high-level waste liquid glass, comprises 1.03-3.13% of BaO by mass, and preferably 1.5-2.5% of BaO by mass.
The starting glass for the joule heating ceramic electric melting furnace suitable for solidifying the power stack high-level waste liquid glass provided by the invention comprises 0.2-2.3% of V by mass percent 2 O 5 Preferably 1 to 2%.
The starting glass for the joule heating ceramic electric melting furnace suitable for solidifying the power stack high-level waste liquid glass provided by the invention comprises 0.3-2% of Sb by mass percent 2 O 5 Preferably 0.8 to 1.8%.
The starting glass for the joule heating ceramic electric melting furnace suitable for solidifying the power stack high-level waste liquid glass provided by the invention comprises ZrO with the mass percentage of 1-3% 2 Preferably 1.5 to 2.5%.
The invention provides a starting glass for a joule heating ceramic electric melting furnace for solidifying power stack high-level waste liquid glass, which comprises La with mass percent of 3-6% 2 O 3 Preferably 5 to 6%.
The starting glass for the joule heating ceramic electric melting furnace suitable for solidifying the power stack high-level waste liquid glass provided by the invention comprises 0.3-1.8% of CeO by mass percent 2 Preferably 0.8 to 1.6%.
The starting glass for the joule heating ceramic electric melting furnace suitable for solidifying the power stack high-level waste liquid glass provided by the invention comprises 1-2.8% of MoO by mass percent 3 Preferably 1.5 to 2.5%.
The invention also provides a preparation method of the starting glass for the joule heating ceramic electric melting furnace, which is suitable for curing the power stack high-level waste liquid glass and comprises the following steps of:
grinding and mixing the components to obtain mixed powder;
and (3) sequentially melting and pouring the mixed powder to obtain the starting glass for the joule heating ceramic electric melting furnace, which is suitable for solidifying the power stack high-level waste liquid glass.
The invention grinds and mixes the components to obtain mixed powder.
The parameters of the grinding and mixing are not particularly limited, so long as the materials can be fully mixed. After the grinding and mixing, the invention preferably further comprises sieving, wherein the sieving times are preferably 3 times.
After the mixed powder is obtained, the mixed powder is sequentially melted and poured to obtain the starting glass for the joule heating ceramic electric melting furnace, which is suitable for solidifying the power stack high-level waste liquid glass.
In the present invention, the melting temperature is preferably 1150 to 1300 ℃, and the time is preferably 3 to 5 hours.
The invention does not limit the property of the starting glass for the joule heating ceramic electric melting furnace, which is obtained by pouring and is suitable for solidifying the power stack high-level waste liquid glass, and the starting glass can be set according to actual conditions; the method comprises the following steps: when the starting glass is applied to the starting of a joule heating ceramic electric melting furnace for solidifying the power stack high-level waste liquid glass, preferably casting into micro-beads, wherein the particle size of the micro-beads starting glass is preferably 0.5-5 mm; when the starting glass is used for performance test, the starting glass is preferably poured into a block shape and then annealed; the annealing treatment temperature is preferably 450-550 ℃, and the heat preservation time is preferably 1.5-3 h.
The invention also provides the application of the starting glass for the joule heating ceramic electric melting furnace for curing the power stack high-level waste liquid glass or the starting glass for the joule heating ceramic electric melting furnace for curing the power stack high-level waste liquid glass, which is obtained by the preparation method of the technical scheme, in the treatment of the power stack high-level waste liquid.
In the invention, the power stack high-level discharge waste liquid contains forty components, mainly contains alkali metal, lanthanide and fission elements (30-70 elements), wherein Al 2 O 3 The content is 5-20wt%; yellow phase "The total content of elemental sulfur, molybdenum and the like is lower and less than 2wt percent; the total content of noble metals Ru, rh, pd, etc. is less than 3wt%.
The invention is not particularly limited in the operation of applying the starting glass for the joule heating ceramic electric melting furnace for curing the power stack high level waste liquid glass to the treatment of the power stack high level waste liquid, and the starting glass can be set according to actual conditions.
The starting glass for a joule heating ceramic electric melting furnace for solidifying a power stack high level waste liquid glass, and the preparation and application thereof, provided by the present invention, will be described in detail with reference to examples, but they should not be construed as limiting the scope of the present invention.
The starting glass compositions in the examples and comparative examples are shown in Table 1.
Table 1 components of starting glass in examples and comparative examples
Sequence number Oxide compound Example 1 Example 2 Example 3 Example 4 Comparative example
1 SiO 2 35 55 47 52 40
2 B 2 O 3 15 12 11 12 11
3 Na 2 O 14 11 8 6 15
4 Li 2 O 3 1.47 2.01 2.52 3.2
5 Al 2 O 3 6 3 5.3 4.2 3.5
6 CaO 8.3 5 7.5 6.8 9
7 MgO 2.08 0.3 1.5 1.8 2.5
8 BaO 2.02 3.13 1.99 1.58 2.5
9 V 2 O 5 2.3 0.2 1.9 1.6 1.1
10 Sb 2 O 5 2 0.3 1.8 1.6 1.2
11 ZrO 2 3 1 2.3 1.6 1.6
12 La 2 O 3 6 3 5.7 5.2 4.7
13 CeO 2 0.3 1.8 1.6 1.2 1.5
14 MoO 3 1 2.8 2.4 1.9 3.2
Totalizing 100 100 100 100 100
The preparation method of the starting glass for the joule heating ceramic electric melting furnace for solidifying the power stack high-level waste liquid glass comprises the following steps:
1) The materials were weighed according to the formulation of table 1 and the total weight was summed up, ground, mixed, and sieved three times to thoroughly mix the materials.
2) Placing the uniformly mixed batch into a platinum crucible, then placing the crucible into a high-temperature furnace, charging for multiple times, melting at a high temperature of 1300 ℃, clarifying for 5 hours, stirring with a stainless steel fine rod, casting into glass blocks after the melting is finished, and annealing for 3 hours at 500 ℃ to obtain block-shaped starting glass for performance test.
The resistivity of the bulk starting glass was measured by GB/T41708-2022 method, the viscosity of the bulk starting glass was measured by ASTM C965-96 method, the crystallization rate of the bulk starting glass was measured by JY/T0587-2020 method, the liquidus line of the bulk starting glass was measured by ASTM C829-81 (2010) method, and the element leaching rate of the bulk starting glass was measured by EJ 1186-2005 and ASTM 1220-17 methods, and the results are shown in Table 2.
Table 2 results of performance test of starting glass obtained in examples and comparative examples
As can be seen from table 2: the resistivity, viscosity and liquidus of the starting glass can meet the operation requirement of the electric melting furnace of the Joule heating ceramic, the operation basic technological performance of the electric melting furnace of the Joule heating ceramic can be ensured, and the crystallization rate and the element leaching rate of the starting glass can ensure that a glass sample is stable for a long time in the deep geological treatment process.
The foregoing is merely a preferred embodiment of the present invention and it should be noted that modifications and adaptations to those skilled in the art may be made without departing from the principles of the present invention, which are intended to be comprehended within the scope of the present invention.

Claims (4)

1. The starting glass for the joule heating ceramic electric melting furnace for solidifying the power stack high-level waste liquid glass is characterized by comprising the following components in percentage by mass:
SiO 2 35~55%,B 2 O 3 9~15%,Na 2 O 6~14%,Li 2 O 1~3%,Al 2 O 3 3~6%,CaO 5~8.3%,MgO 0.3~2.08%,BaO 1.03~3.13%,V 2 O 5 0.2~2.3%,Sb 2 O 5 0.3~2%,ZrO 2 1~3%,La 2 O 3 3~6%,CeO 2 0.3~1.8%,MoO 3 1~2.8%。
2. the method for preparing starting glass for a joule-heated ceramic electric furnace for solidifying power stack high level waste liquid glass as claimed in claim 1, comprising the steps of:
grinding and mixing the components to obtain mixed powder;
and (3) sequentially melting and pouring the mixed powder to obtain the starting glass for the joule heating ceramic electric melting furnace, which is suitable for solidifying the power stack high-level waste liquid glass.
3. The method according to claim 2, wherein the melting temperature is 1150-1300 ℃ for 3-5 hours.
4. The use of the starting glass for a joule-heated ceramic electric furnace for curing a power stack spent liquor glass according to claim 1 or the starting glass for a joule-heated ceramic electric furnace for curing a power stack spent liquor glass obtained by the preparation method according to claim 2 or 3 for treating a power stack spent liquor.
CN202311650282.5A 2023-12-05 2023-12-05 Starting glass for joule heating ceramic electric melting furnace suitable for solidifying power stack high-level waste liquid glass, and preparation and application thereof Pending CN117658462A (en)

Priority Applications (1)

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CN202311650282.5A CN117658462A (en) 2023-12-05 2023-12-05 Starting glass for joule heating ceramic electric melting furnace suitable for solidifying power stack high-level waste liquid glass, and preparation and application thereof

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CN202311650282.5A CN117658462A (en) 2023-12-05 2023-12-05 Starting glass for joule heating ceramic electric melting furnace suitable for solidifying power stack high-level waste liquid glass, and preparation and application thereof

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