Selenite Sorption on Hydrated CEM-V/A Cement in the Presence of Steel Corrosion Products: Redox vs Nonredox Sorption
- 23 January 2020
- journal article
- research article
- Published by American Chemical Society (ACS) in Environmental Science & Technology
- Vol. 54 (4), 2344-2352
- https://doi.org/10.1021/acs.est.9b06876
Abstract
Reinforced cementitious structures in nuclear waste repositories will act as barriers that limit the mobility of radionuclides (RNs) in case of eventual leakage. CEM-V/A cement, a ternary blended cement with blast furnace slag (BFS) and fly ash (FA) could be qualified and used in nuclear waste disposal. Chemical interactions between the cement and RNs are critical but not completely understood. Here, we combined wet chemistry methods, synchrotron-based X-ray techniques, and thermodynamic modelling to explore the redox interactions and non-redox sorption processes in simulated steel-reinforced CEM-V/A hydration systems using selenite as a molecular probe. Among all the steel corrosion products analysed, only the addition of Fe0 can obviously enhance the reducing ability of cement towards selenite. In comparison, steel corrosion products showed stronger reducing power in the absence of cement hydrates. Sele-nium K-edge X-ray absorption spectroscopy (XAS) revealed that selenite immobilization mechanisms included non-redox inner-/outer-sphere complexations and reductive precipita-tions of FeSe and/or Se(0). Importantly, the hydrated pristine cement showed a good reducing ability, driven by ferrous phases and (bi)sulfides (as shown by sulfur K-edge XAS) originated from BFS and FA. The overall redox potential imposed by hydrated CEM-V/A was deter-mined, hinting to a redox shift in underground cementitious structures.Keywords
Funding Information
- Labex (ANR10 LABX56)
- China Scholarship Council
- Agence Nationale pour la Gestion des D?chets Radioactifs
This publication has 43 references indexed in Scilit:
- A review of the retention mechanisms of redox-sensitive radionuclides in multi-barrier systemsApplied Geochemistry, 2018
- Deciphering mineralogical changes and carbonation development during hydration and ageing of a consolidated ternary blended cement pasteIUCrJ, 2018
- Calcium silicate hydrates: Solid and liquid phase compositionCement and Concrete Research, 2015
- The evolution of clay rock/cement interfaces in a cementitious repository for low- and intermediate level radioactive wastePhysics and Chemistry of the Earth, Parts A/B/C, 2013
- Structural Insight into Iodide Uptake by AFm PhasesEnvironmental Science & Technology, 2012
- Preparation of radiochemically pure 79Se and highly precise determination of its half-lifeApplied Radiation and Isotopes, 2010
- Binding mechanisms of radionuclides to cementCement and Concrete Research, 2008
- Thermodynamic properties of Portland cement hydrates in the system CaO–Al2O3–SiO2–CaSO4–CaCO3–H2OCement and Concrete Research, 2007
- The AFm phase in Portland cementCement and Concrete Research, 2007
- Dissolution-precipitation behaviour of ettringite, monosulfate, and calcium silicate hydrateCement and Concrete Research, 2003