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Sub-nanometer Resolution Imaging with Amplitude-modulation Atomic Force Microscopy in Liquid

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Structural insight into iodide uptake by AFm phases.

Laure Aimoz¹, Erich Wieland, Christine Taviot-Guého

¹Laboratory for Waste Management, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland. laure.aimoz@psi.ch

Environmental Science & Technology

|March 2, 2012

Summary

Calcium-monosulfate (AFm-SO(4)) effectively retards iodide mobility in cement phases, crucial for radioactive waste disposal. This phase shows potential for immobilizing iodine-129 in groundwater, enhancing safety measures.

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Area of Science:

Geochemistry
Materials Science
Environmental Science

Background:

Radioactive waste disposal requires immobilizing mobile contaminants like iodide (I(-)).
Cementitious materials are considered for radioactive waste containment.
Positively charged cement phases' ability to sorb anions is key to contaminant retardation.

Purpose of the Study:

Investigate the retardation of iodide (I(-)) mobility by cement phases.
Identify specific cement phases capable of sequestering iodide.
Understand the structural mechanisms behind iodide uptake in AFm phases.

Main Methods:

Sorption experiments using iodine-125 ((125)I) on various AFm phases (ettringite, hydrotalcite, chloride-, carbonate-, and sulfate-containing).
Structural analysis using X-ray diffraction (XRD) for AFm phase characterization.
Extended X-ray absorption fine structure (EXAFS) spectroscopy to probe iodine's coordination environment.

Main Results:

Calcium-monosulfate (AFm-SO(4)) was the only phase that sorbed trace levels of iodide.
XRD revealed solid solution formation between AFm-I(2) and AFm-SO(4) in I-SO(4) mixtures.
EXAFS indicated modified iodine coordination in I-CO(3) and I-SO(4) samples, suggesting structural changes and potential for retardation.

Conclusions:

AFm-SO(4) demonstrates significant potential for retarding (129)I mobility due to solid solution formation with iodide.
The uptake mechanism involves structural incorporation and modification of iodine's coordination environment.
Findings support the use of specific cement phases for enhancing radioactive waste isolation.