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Iodine speciation in a silver-amended cementitious system.

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PubMed
Summary

Disposing of silver-impregnated zeolite (AgIZ) in slag-free grout effectively immobilizes iodine and silver. Slag-containing grout, however, fails to immobilize iodine due to reductive conditions, leading to significant release.

Keywords:
CementImmobilizationIodine speciationRedoxSilver-impregnated zeoliteSlag

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Area of Science:

  • Environmental Science and Engineering
  • Geochemistry
  • Materials Science

Background:

  • Silver-impregnated zeolite (AgIZ) is crucial for removing radioiodine from nuclear waste streams.
  • The increasing inventory of AgIZ waste necessitates effective and safe disposal methods.
  • Grout waste forms are commonly used for low-level radioactive waste disposal.

Purpose of the Study:

  • To evaluate the efficacy of two distinct grout waste forms (slag-free and slag-containing) for immobilizing iodine (I) and silver (Ag) from used AgIZ.
  • To determine the iodine speciation leached from AgIZ encapsulated within these grout matrices.
  • To assess the impact of grout composition and redox conditions on iodine immobilization and potential release.

Main Methods:

  • A 60-day kinetics batch leaching experiment was conducted with AgIZ encapsulated in slag-free and slag-containing grouts.
  • Analysis of leached iodine (Itotal) concentrations in the contact solutions.
  • Thermodynamic calculations to understand redox conditions (Eh) and their influence on iodine speciation.
  • Iodine K-edge X-ray absorption near edge structure (XANES) analysis to identify iodine species.

Main Results:

  • Slag-free grout demonstrated excellent immobilization of I and Ag, releasing only 3.3 μg/L Itotal.
  • Slag-containing grout was ineffective, releasing a significantly higher 19,269 μg/L Itotal due to reductive dissolution of silver iodide (AgI).
  • Reducing conditions (Eh = -392 mV) in slag-containing grout promoted iodide (I-) release, while oxidizing conditions (Eh = 439 mV) in slag-free grout limited release.
  • Leached iodine primarily existed as iodide (I-) and organo-iodine (org-I), with minimal iodate detected in both systems.

Conclusions:

  • Subsurface disposal of AgIZ waste requires oxidizing conditions to ensure effective iodine immobilization.
  • The choice of grout matrix significantly impacts the immobilization of iodine and silver from AgIZ.
  • Reductive conditions in slag-containing grout can lead to the release of radioiodide, necessitating careful consideration of disposal environments and potential speciation transformations.