Thermodynamics, kinetics, and mechanics of cesium sorption in cement paste: A multiscale assessment

Jack Arayro, Alice Dufresne, Tingtao Zhou, Katerina Ioannidou, Josef-Franz Ulm, Roland Pellenq, and Laurent Karim Béland
Phys. Rev. Materials 2, 053608 – Published 30 May 2018
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Abstract

Cesium-137 is a common radioactive byproduct found in nuclear spent fuel. Given its 30 year half life, its interactions with potential storage materials—such as cement paste—is of crucial importance. In this paper, simulations are used to establish the interaction of calcium silicate hydrates (C-S-H)—the main binding phase of cement paste—with Cs at the nano- and mesoscale. Different C-S-H compositions are explored, including a range of Ca/Si ratios from 1.0 to 2.0. These calculations are based on a set of 150 atomistic models, which qualitatively and quantitatively reproduce a number of experimentally measured features of C-S-H—within limits intrinsic to the approximations imposed by classical molecular dynamics and the steps followed when building the models. A procedure where hydrated Ca2+ ions are swapped for Cs1+ ions shows that Cs adsorption in the C-S-H interlayer is preferred to Cs adsorption at the nanopore surface when Cs concentrations are lower than 0.19 Mol/kg. Interlayer sorption decreases as the Ca/Si ratio increases. The activation relaxation technique nouveau is used to access timescales out of the reach of traditional molecular dynamics (MD). It indicates that characteristic diffusion time for Cs1+ in the C-S-H interlayer is on the order of a few hours. Cs uptake in the interlayer has little impact on the elastic response of C-S-H. It leads to swelling of the C-S-H grains, but mesoscale calculations that access length scales out of the range of MD indicate that this leads to practically negligible expansive pressures for Cs concentrations relevant to nuclear waste repositories.

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  • Received 6 December 2017
  • Corrected 18 August 2023

DOI:https://doi.org/10.1103/PhysRevMaterials.2.053608

©2018 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Corrections

18 August 2023

Correction: The omission of a second affiliation for the first author has been set right. This change necessitated renumbering of the subsequent affiliations.

Authors & Affiliations

Jack Arayro1,2, Alice Dufresne3, Tingtao Zhou4, Katerina Ioannidou1,3, Josef-Franz Ulm3, Roland Pellenq1,3,5, and Laurent Karim Béland1,6,*

  • 1MultiScale Materials Science for Energy and Environment (MSE2), The Joint CNRS/MIT/Aix-Marseille University Laboratory, UMI CNRS 3466, Massachusetts Institute of Technology, Cambridge, MIT 02139, Massachusetts, USA
  • 2College of Engineering and Technology, American University of the Middle East, Eqaila 54200, Kuwait
  • 3Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, Queen's K7L 3N6, Massachusetts, USA
  • 4Department of Physics, Massachusetts Institute of Technology, Cambridge, Massachusetts, USA
  • 5CINaM-Aix Marseille Université-CNRS, Marseille, France
  • 6Department of Mechanical and Materials Engineering, Queen's University, Kingston, Ontario, Canada

  • *laurent.beland@queensu.ca

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Issue

Vol. 2, Iss. 5 — May 2018

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