The evolution of hydrated lime-based cementitious waste forms during leach testing leading to enhanced technetium retention

The interaction between radionuclides and cementitious material phases is crucial in the prediction of the long-term disposal behavior of cementitious waste forms. This work focuses on the behavior of technetium-99 (Tc) within a hydrated-lime based waste form developed as a candidate to immobilize h...

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Veröffentlicht in:Journal of hazardous materials 2022-05, Vol.430 (C), p.128507-128507, Article 128507
Hauptverfasser: Bourchy, Agathe, Saslow, Sarah A., Williams, Benjamin D., Avalos, Nancy M., Um, Wooyong, Canfield, Nathan L., Sweet, Lucas, Smith, Gary L., Asmussen, R. Matthew
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container_end_page 128507
container_issue C
container_start_page 128507
container_title Journal of hazardous materials
container_volume 430
creator Bourchy, Agathe
Saslow, Sarah A.
Williams, Benjamin D.
Avalos, Nancy M.
Um, Wooyong
Canfield, Nathan L.
Sweet, Lucas
Smith, Gary L.
Asmussen, R. Matthew
description The interaction between radionuclides and cementitious material phases is crucial in the prediction of the long-term disposal behavior of cementitious waste forms. This work focuses on the behavior of technetium-99 (Tc) within a hydrated-lime based waste form developed as a candidate to immobilize high-sulphate containing liquid wastes known to inhibit cement solidification when using a fly ash based formulation. In leach testing, the hydrated-lime based formulation demonstrated improvement in Tc retention over a fly ash containing formulation beginning after 14 d leaching. The mineralogical evolution of the hydrated-lime samples during leach testing showed a decrease in portlandite content and reduction capacity at the onset of the Tc retention improvement. Leach testing upwards of 400 days showed the improved Tc retention was sustained. Samples cured for different lengths of time (28 days vs 60 days) confirmed that the improved Tc retention and mineralogic change was caused by cement – leachant interactions and not the sample curing time. The Tc observed diffusivities in the hydrated-lime samples are amongst the lowest measured in a cement waste form tested for development at the US Department of Energy Hanford site, leading to a possible pathway to improved cement conditioning where contaminants can be retained for long disposal times. [Display omitted] •Hydrated lime (HL) cement formula solidifies high sulphate nuclear waste simulant.•Tc diffusivity lowered by early Tc(VII) reduction to stable Tc(IV) phases.•Reoxidized TcO4- may be incorporated into mineral phases during aqueous leaching.•Tc retention observed is among the lowest in Hanford Site-relevant waste forms.
doi_str_mv 10.1016/j.jhazmat.2022.128507
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subjects Chemical Sciences
Diffusivity
Material chemistry
Mineralogical incorporation
Nuclear waste
Reduction capacity
title The evolution of hydrated lime-based cementitious waste forms during leach testing leading to enhanced technetium retention
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