A kind of low temperature preparation method of strontium and cesium glass ceramic co-solidified body

A technology of glass ceramics and solidified body, which is applied in radioactive purification, nuclear engineering, etc., can solve the problems of simultaneous solidification of strontium and cesium, does not involve the evaluation of leaching resistance of solidified nuclides, and high cost of industrial application, so as to solve the problem of solidification of ceramics Strong element selectivity, solution to unsatisfactory packaging capacity, and high mechanical stability

Active Publication Date: 2022-07-01
SOUTHWEAT UNIV OF SCI & TECH
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  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, most single-phase ceramic substrates have strong selectivity to radionuclides, and often can only contain a single and limited radionuclides, and cannot achieve simultaneous curing of strontium and cesium, and the cost of later industrial applications is high.
In addition, the preparation method of the ceramic solidified body is mainly a high-temperature solid-state reaction method. The process is to contact the solid-phase reactants with each other, and to prepare the target through the process of contact surface and phase region diffusion, migration, crystal nucleus formation and nucleus growth. The product generally has a high synthesis temperature (~1400-1500°C) and a long preparation time (>48h), and it is easy to form a heterogeneous phase during the synthesis process, which will cause the volatilization of cesium
For example, a master's degree thesis was published in 2005 (Zhao Yulong, China Institute of Atomic Energy, "Man-made rock solidification simulation 90Sr, 137Cs nuclide waste research"), the thesis uses the mineral phase combination of manganite, perovskite and rutile , conducted a simultaneous ceramic solidification study on strontium and cesium, and found that the solidified body has a dense structure and a low strontium and cesium leaching rate; but the hot-pressing sintering temperature of the ceramic solidified body is 1200 ° C, which will inevitably lead to the volatilization of a large amount of cesium
The Chinese invention patent application with publication number 102208223B in 2011 discloses a method for preparing a strontium-cesium co-solidified body. The method is based on modified ZSM-5A molecular sieve, and is absorbed in the solution, evaporated and dried, and calcined by temperature programming. Finally, strontium and cesium solidified polycrystals were obtained, which realized the simultaneous and low-temperature solidification of strontium and cesium, and solved the volatilization problem of cesium; Evaluation of leaching resistance of polycrystalline bonding, molding and curing nuclides

Method used

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  • A kind of low temperature preparation method of strontium and cesium glass ceramic co-solidified body
  • A kind of low temperature preparation method of strontium and cesium glass ceramic co-solidified body
  • A kind of low temperature preparation method of strontium and cesium glass ceramic co-solidified body

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Experimental program
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Effect test

Embodiment 1

[0027] A low-temperature preparation method of strontium and cesium glass-ceramic co-solidified body is characterized in that, comprises the following steps:

[0028] Step 1, take the Ba(NO 3 ) 2 , Sr(NO 3 ) 2 , CsNO 3 , La(NO 3 ) 3 ·6H 2 O and Zr (NO 3 ) 2 ·5H 2 O was added to deionized water, and stirred at a speed of 300 r / min until dissolved; the deionized water was mixed with Zr(NO) 3 ) 2 ·5H 2 The molar ratio of O is 600:1;

[0029] Step 2: Add citric acid to the stirred solution in step 1, and stir and chelate for 1 hour at a speed of 300 r / min; the citric acid and Ba(NO) 3 ) 2 , Sr(NO 3 ) 2 , CsNO 3 , La(NO 3 ) 3 ·6H 2 O and Zr (NO 3 ) 2 ·5H 2 The molar ratio of the total cations of O is 3:1;

[0030] Step 3, adding acrylamide to the solution after stirring and chelating in step 2, and then stirring at a speed of 300 r / min at 75° C. to obtain a transparent gel; the acrylamide and Ba(NO) 3 ) 2 , Sr(NO 3 ) 2 , CsNO 3 , La(NO 3 ) 3 ·6H 2 O ...

Embodiment 2

[0035] A low-temperature preparation method of strontium and cesium glass-ceramic co-solidified body is characterized in that, comprises the following steps:

[0036] Step 1, take the Ba(NO 3 ) 2 , Sr(NO 3 ) 2 , CsNO 3 , La(NO 3 ) 3 ·6H 2 O and Zr (NO 3 ) 2 ·5H 2 O was added to deionized water, and stirred at a speed of 250 r / min until dissolved; the deionized water was mixed with Zr(NO) 3 ) 2 ·5H 2 The molar ratio of O is 700:1;

[0037] Step 2. Add glucono-δ-lactone to the stirred solution in step 1, and stir and chelate at a speed of 250r / min for 1.5h; the glucono-δ-lactone and Ba(NO) 3 ) 2 , Sr(NO 3 ) 2 , CsNO 3 , La(NO 3 ) 3 ·6H 2 O and Zr (NO 3 ) 2 ·5H 2 The molar ratio of the total cations of O is 4:1;

[0038] Step 3, adding polyvinyl alcohol to the solution after stirring and chelating in step 2, and then stirring at a speed of 200 r / min at 80 ° C to obtain a transparent gel; the polyvinyl alcohol and Ba(NO) 3 ) 2 , Sr(NO 3 ) 2 , CsNO 3 , ...

Embodiment 3

[0043] A low-temperature preparation method of strontium and cesium glass-ceramic co-solidified body is characterized in that, comprises the following steps:

[0044] Step 1, take the Ba(NO 3 ) 2 , Sr(NO 3 ) 2 , CsNO 3 , La(NO 3 ) 3 ·6H 2 O and Zr (NO 3 ) 2 ·5H 2 O was added to deionized water, and stirred at a speed of 250 r / min until dissolved; the deionized water was mixed with Zr(NO) 3 ) 2 ·5H 2 The molar ratio of O is 700:1;

[0045] Step 2. Add glucono-δ-lactone to the stirred solution in step 1, and stir and chelate at a speed of 250r / min for 1.5h; the glucono-δ-lactone and Ba(NO) 3 ) 2 , Sr(NO 3 ) 2 , CsNO 3 , La(NO 3 ) 3 ·6H 2 O and Zr (NO 3 ) 2 ·5H 2 The molar ratio of the total cations of O is 4:1;

[0046] Step 3, adding polyvinyl alcohol to the solution after stirring and chelating in step 2, and then stirring at a speed of 200 r / min at 80 ° C to obtain a transparent gel; the polyvinyl alcohol and Ba(NO) 3 ) 2 , Sr(NO 3 ) 2 , CsNO 3 , ...

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Abstract

The invention discloses a low-temperature preparation method of a strontium and cesium glass ceramic co-solidified body, comprising: taking Ba(NO 3 ) 2 , Sr(NO 3 ) 2 , CsNO 3 , La(NO 3 ) 3 ·6H 2 O and Zr (NO 3 ) 2 ·5H 2 Add O into deionized water and stir until dissolved; add a chelating agent to the stirred solution, stir and chelate; add a gelling agent to the stirred chelated solution, and stir to obtain a transparent gel; the prepared transparent gel Drying, then heat treatment to obtain a black powder precursor; heat treatment of the black powder precursor to obtain a polycrystalline solidified body, the solidified body is mixed with a glass binder, and then pressed into a block by a hydraulic press, and the obtained block is calcined to make the polycrystalline solidified body. The crystalline solidified body powder is wrapped in a glass phase matrix to make a strontium and cesium glass-ceramic co-solidified body with high mechanical stability and low leaching resistance.

Description

technical field [0001] The invention relates to the technical field of solidification of radionuclide fission products, in particular to a low-temperature preparation method of a co-solidified body of strontium and cesium glass ceramics. Background technique [0002] Strontium and cesium are the two most important heat sources for the generation of radionuclide fission products in high-level waste liquids during the development and utilization of nuclear energy. The impact cannot be ignored. At present, the industrial treatment of strontium and cesium is mainly glass curing. Although its glass solidified body has the advantages of good resistance to β and γ radiation and strong tolerance, but glass is a metastable phase after all, with poor thermodynamic stability and resistance to α radiation. At low temperature, devitrification or crystallization is easy to occur, which leads to cracks in the solidified body, which increases the leaching rate of nuclides; in addition, a ...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C03C10/02C03C6/00C03B32/02C04B35/48C04B35/626G21F9/16
CPCC03C10/0063C04B35/48C04B35/62605C03B32/02G21F9/162C04B2235/3201C04B2235/3215C04B2235/3213C04B2235/3227
Inventor 刘海峰赵键张行泉霍冀川郑奎
Owner SOUTHWEAT UNIV OF SCI & TECH
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