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Method for treating radioactive waste liquid by using phosphate minerals

A radioactive waste liquid, phosphate technology, applied in radioactive purification, nuclear engineering and other directions, can solve the problems of unfavorable engineering application, large thermal expansion coefficient and strong corrosion, small solid solution, etc., achieve excellent structural flexibility, improve Long-term safety, effect of low structural symmetry

Inactive Publication Date: 2021-07-16
SOUTHWEAT UNIV OF SCI & TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

At present, the vitrification technology also has the following problems: (1) the amount of solid solution of high-level radioactive waste, especially actinide nuclides, in silicate glass is small, generally lower than 4wt.%. Phosphate glass has a low melting temperature. , High waste containment capacity, etc., but it has a large thermal expansion coefficient and strong corrosiveness, which is not conducive to engineering applications; (2) Glass is a metastable phase, and in high temperature and humid environments, the glass phase will corrode, crystallize or Fragmentation causes the leaching rate of nuclide to increase rapidly, and the vitrified body cannot meet the requirements of geological disposal after 1000 years
Vitrification in the solidification technology has strong adaptability to waste source items, and is the only treatment technology for high-level radioactive waste that has been applied in engineering. However, glass is a metastable phase, and vitrification containing actinide nuclides is difficult to meet the long-term requirements of geological disposal. Safety requirements: The cured body prepared by ceramic solidification has good long-term safety, but has poor adaptability to waste sources with complex components, and it is difficult to directly and safely solidify actinide nuclides in high-level waste liquid

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0067] to La 3+ To simulate the trivalent actinide nuclides, LaCl 3 ·7H 2 O is a raw material, by adding an appropriate amount of water in a hydrothermal reactor, prepare 200ml simulated trivalent actinide nuclides (La 3+ ) waste liquid, the design formula is Ce 1-x La x PO 4 0.667H 2 O(03 ·7H 2 O, NH 4 h 2 PO 4 Raw material, control 03 ·7H 2 O:CeCl 3 ·7H 2 O≤1 (molar ratio), NH 4 h 2 PO 4 :(CeCl 3 ·7H 2 O+LaCl 3 ·7H 2 O)=1.01:1 (molar ratio), Ce 3+ and La 3+ The molar concentration of ions (C) is C(Ce 3+ )+C(La 3+ )=0.001mol / L; under conditions of 60°C temperature, pH value 0.3, and time of 4 days, Ce 1-x La x PO 4 0.667H 2 O(01-x La x PO 4 Monazite ceramic solidified body; the green body after heat treatment is sintered in a vacuum hot-pressed sintering furnace at 1150°C and 30MPa for 120 minutes to obtain Ce with good sintering, relative density exceeding 98%, and excellent performance. 1-x La x PO 4 Monazite ceramic solidified body.

Embodiment 2

[0069] to La 3+ To simulate the trivalent actinide nuclides, LaCl 3 ·7H 2 O is a raw material, by adding an appropriate amount of water in a hydrothermal reactor, prepare 200ml simulated trivalent actinide nuclides (La 3+ ) waste liquid, the design formula is Ce 1-x La x PO 4 0.667H 2 O(03 ·7H 2 O, NH 4 h 2 PO 4 Raw material, control 03 ·7H 2 O:CeCl 3 ·7H 2 O≤1 (molar ratio), NH 4 h 2 PO 4 :(CeCl 3 ·7H 2 O+LaCl 3 ·7H 2 O)=1.05:1 (molar ratio), Ce 3+ and La 3+ The molar concentration of ions (C) is C(Ce 3+ )+C(La 3+ )=0.001mol / L; under conditions of 60°C temperature, pH value 0.3, and time of 4 days, Ce 1-x La x PO 4 0.667H 2 O(01-x La x PO 4 Monazite ceramic solidified body; the green body after heat treatment is sintered in a vacuum hot-pressed sintering furnace at 1150°C and 30MPa for 120 minutes to obtain Ce with good sintering, relative density exceeding 98%, and excellent performance. 1-x La x PO 4 Monazite ceramic solidified body.

Embodiment 3

[0071] to La 3+ To simulate the trivalent actinide nuclides, LaCl 3 ·7H 2 O is a raw material, by adding an appropriate amount of water in a hydrothermal reactor, prepare 200ml simulated trivalent actinide nuclides (La 3+ ) waste liquid, the design formula is Ce 1-x La x PO 4 0.667H 2 O(03 ·7H 2 O, NH 4 h 2 PO 4 Raw material, control 03 ·7H 2 O:CeCl 3 ·7H 2 O≤1 (molar ratio), NH 4 h 2 PO 4 :(CeCl 3 ·7H 2 O+LaCl 3 ·7H 2 O)=1.1:1 (molar ratio), Ce 3 + and La 3+ The molar concentration of ions (C) is C(Ce 3+ )+C(La 3+ )=0.001mol / L; under conditions of 60°C temperature, pH value 0.3, and time of 4 days, Ce 1-x La x PO 4 0.667H 2 O(01-x La x PO 4 Monazite ceramic solidified body; the green body after heat treatment is sintered in a vacuum hot-pressed sintering furnace at 1150°C and 30MPa for 120 minutes to obtain Ce with good sintering, relative density exceeding 98%, and excellent performance. 1-x La x PO 4 Monazite ceramic solidified body.

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PUM

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Abstract

The invention discloses a method for treating radioactive waste liquid through phosphate minerals. The method comprises the following steps: by simulating trivalent actinide nuclides by using trivalent lanthanide elements, simulating tetravalent actinide nuclides by using Th 4+, taking LaCl3.7H2O, CeCl3.7H2O, PrCl3.6H2O, NdCl3.6H2O, SmCl3.6H2O, EuCl3.6H2O, GdCl3.6H2O, NH4H2PO4, Th(NO3)4.4H2O, CaCl2 and SrCl2.6H2O as raw materials, enriching the simulated actinide nuclides by using CePO4.0.667H2O and cerite precipitates, preparing a MyThyCe(1-x-2y)LnxPO4 monazite ceramic solidified body through solid-phase sintering. By means of the method, efficient volume reduction of the high-level liquid waste and safe lattice solidification treatment of the actinide nuclides can be achieved, and the high-level liquid waste can be safely treated and disposed.

Description

technical field [0001] The invention belongs to the solidification treatment of radioactive waste liquid, and relates to a method for treating radioactive waste liquid with phosphate minerals. The invention is particularly suitable for the safe treatment and disposal of high-level radioactive waste liquid containing actinide nuclides. Background technique [0002] With the increase in energy demand and the improvement of environmental protection awareness, nuclear energy is still the preferred energy source in terms of resources, economy, and safety, but the radioactive waste generated restricts the sustainable development of nuclear energy. Therefore, how to safely and effectively dispose of radioactive waste is a domestic issue. external problems. High-level liquid waste (referred to as HLLW, High-level liquid waste in English) is derived from the extract produced by the uranium-plutonium co-decontamination cycle in the PUREX (Plutonium Uranium Redox Extraction) process o...

Claims

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Application Information

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IPC IPC(8): C04B35/447C04B35/50C04B35/622C04B35/645G21F9/16
CPCC04B35/447C04B35/50C04B35/62204C04B35/645C04B2235/3224C04B2235/3227C04B2235/3229G21F9/162
Inventor 赵骁锋滕元成郑夏宇刘航李玉香吴浪王山林
Owner SOUTHWEAT UNIV OF SCI & TECH
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