Metakaolin Silicate Additives for Cesium Vitrification

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Solution Overview

Problem

The existing vitrification processes for cesium radionuclides, particularly 137Cs, face challenges in minimizing evaporation during the high-temperature melting process, leading to inefficiencies and increased reprocessing needs, which affects the economic and long-term safety of radioactive waste immobilization.

Innovation Solution

The use of additives based on metakaolin and anhydrous sodium or potassium silicate, which undergo exothermic polycondensation reactions to form a three-dimensional amorphous structure, effectively immobilizing cesium radionuclides over the entire temperature range of the vitrification process, preventing crystallization and maintaining high chemical resistance.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If high temperature melting (above 1400°C) is used to produce glass matrices, then the glass achieves high chemical resistance and stability, but radionuclides volatilize from the melting mixture creating additional wastes

Engineering Contradiction:
Improvechemical resistanceVSAvoidradionuclide volatilization
Core Design Contradiction:
ReliabilityVSLoss of substance

Solution Approach 1:

The patent introduces a preliminary action by adding specific additives (metakaolin, anhydrous sodium silicate, anhydrous potassium silicate) to the glass matrix before the melting process. These additives undergo exothermic polycondensation reactions that form a three-dimensional amorphous structure capable of retaining radionuclides, preventing their volatilization during subsequent high-temperature processing while maintaining the glass's chemical resistance

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The patent applies parameter changes by modifying the chemical composition of the glass matrix through the addition of specific compounds (metakaolin with SiO2/Al2O3 ratio of 1.34-1.5, anhydrous sodium silicate with SiO2/Na2O ratio of 0.98-1, or anhydrous potassium silicate). These compositional changes enable the formation of a geopolymer structure that retains radionuclides at high temperatures

Inventive Principle:
Principle #35Parameter changes

2Loss of substance

If temperature is reduced below 1400°C to prevent radionuclide evaporation, then volatilization is suppressed, but the glass matrix may crystallize and chemical resistance decreases

Engineering Contradiction:
Improveradionuclide evaporationVSAvoidchemical resistance
Core Design Contradiction:
Loss of substanceVSReliability

Solution Approach 1:

The patent introduces a preliminary action by adding specific additives (metakaolin, anhydrous sodium silicate, anhydrous potassium silicate) to the glass matrix before the melting process. These additives undergo exothermic polycondensation reactions that form a three-dimensional amorphous structure capable of retaining radionuclides, preventing their volatilization during subsequent high-temperature processing while maintaining the glass's chemical resistance

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The patent applies composite materials by creating a geopolymer-based glass matrix that combines metakaolin, anhydrous sodium silicate, and/or anhydrous potassium silicate in specific ratios. This composite structure provides both the low melting point needed to prevent radionuclide evaporation and the chemical resistance required for long-term stability

Inventive Principle:
Principle #40Composite materials

3Quantity of substance

If conventional glass compositions are used, then the glass can absorb radionuclides, but cesium radionuclides still escape during thermal treatment due to low melting temperature and high evaporation tendency

Engineering Contradiction:
Improveradionuclide absorptionVSAvoidcesium volatilization
Core Design Contradiction:
Quantity of substanceVSLoss of substance

Solution Approach 1:

The patent applies parameter changes by modifying the chemical composition of the glass matrix through the addition of specific compounds (metakaolin with SiO2/Al2O3 ratio of 1.34-1.5, anhydrous sodium silicate with SiO2/Na2O ratio of 0.98-1, or anhydrous potassium silicate). These compositional changes enable the formation of a geopolymer structure that retains radionuclides at high temperatures

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent uses metakaolin and anhydrous silicates as intermediary substances that facilitate the retention of cesium radionuclides. These additives undergo polycondensation reactions to form a geopolymer matrix that acts as an intermediary structure, trapping radionuclides within its three-dimensional amorphous network and preventing their escape during thermal treatment

Inventive Principle:
Principle #24Intermediary (Mediator)

Applied Scientific Principles

This section explains which scientific principles are used to turn an abstract innovation direction into a practical engineering solution.

Function Achieved in This Case

This approach significantly reduces cesium radionuclide evaporation and maximizes retention within the glass matrix, achieving 99.96% retention efficiency, ensuring safe and stable long-term storage by maintaining the radionuclides in an amorphous glass phase without crystallization.

Implementation Method 1

additives based on metakaolin and at least one of anhydrous sodium silicate or anhydrous potassium silicate, which undergo exothermic polycondensation reactions

Methodology Applied
Scientific EffectExothermic reaction: Exothermic Reaction

Implementation Method 2

Use of additives for vitrification of liquid radioactive cesium radionuclides-containing wastes

Methodology Applied
Scientific EffectVitrification: Vitrification

Data Source

PatentEP3849950B1Use of additives for vitrification of liquid radioactive cesium radionuclides-containing wastes having high retention efficiency of said radionuclides over the entire range of vitrification temperature
Publication Date: 2022.08.03 VUJE AS
  • EP3849950B1 patent drawingFigure 1
  • EP3849950B1 patent drawingFigure 2

AI summary

The present invention relates to additives for the vitrification of liquid radioactive wastes containing cesium radionuclides, the additives having high retention efficiency of said radionuclides over the entire temperature range of the vitrification process and comprisingmetakaolin and anhydrous sodium silicate and/or anhydrous potassium silicate as ingredients of a homogeneous powder mixture or a dry granulate. The ingredients are in close contact and their grain size is at least on the micron level. The additives can further comprise inorganic hydrophilic materials and/or a fluxing agent. The invention also includes a method of preparing said additives and also use of said additives for immobilisation of cesium radionuclides in the process of vitrification of liquid radioactive waste over the entire temperature range of the vitrification process. Cesium radionuclide is preferably 137Cs radionuclide.