Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study

Sophie Le Caër; Lucile Dezerald; Khaoula Boukari; Maxime Lainé; Sébastien Taupin; Ryan M. Kavanagh; Conrad S.N. Johnston; Eddy Foy; Thibault Charpentier; Konrad J. Krakowiak; Roland J M Pellenq; Franz J. Ulm; Gareth A. Tribello; Jorge Kohanoff; Andres Saúl

doi:10.1016/j.cemconres.2017.05.022

Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study

Sophie Le Caër, Lucile Dezerald, Khaoula Boukari, Maxime Lainé, Sébastien Taupin, Ryan M. Kavanagh, Conrad S.N. Johnston, Eddy Foy, Thibault Charpentier, Konrad J. Krakowiak, Roland J M Pellenq, Franz J. Ulm, Gareth A. Tribello, Jorge Kohanoff, Andres Saúl

School of Mathematics and Physics

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Abstract

Long-term confinement of nuclear waste is one of the main challenges faced by the nuclear industry. Fission products such as ⁹⁰Sr and ¹³⁷Cs, both β− emitters known to induce serious health hazards, represent the largest fraction of nuclear waste. Cement is a good candidate to store them, provided it can resist the effects of irradiation over time. Here, we have investigated the effects of β− decay on cement by performing electron irradiation experiments on different samples. We show that H₂ production in cement, the main effect of water radiolysis, depends strongly on composition and relative humidity. First-principles calculations indicate that the water-rich interlayer regions with Ca²⁺ ions act as electron traps that promote the formation of H₂. They also show that holes localize in water-rich regions in low Ca content samples and are then able to participate in H₂ production. This work provides new understanding of radiolysis effects in cements.

Original language	English
Pages (from-to)	110-118
Number of pages	9
Journal	Cement and Concrete Research
Volume	100
Early online date	15 Jun 2017
DOIs	https://doi.org/10.1016/j.cemconres.2017.05.022
Publication status	Published - Oct 2017

Keywords

Cement paste
Radiolysis
H2 production
First-principles calculations
Reaction mechanisms

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Production of H2 by water radiolysis in cement paste under electron irradiation
Copyright 2017 Elsevier. This manuscript is distributed under a Creative Commons Attribution-NonCommercial-NoDerivs License (https://creativecommons.org/licenses/by-nc-nd/4.0/), which permits distribution and reproduction for non-commercial purposes, provided the author and source are cited.
Accepted author manuscript, 1.98 MBLicence: CC BY-NC-ND

Exploration of Hydrogen Gas Evolution from Radioactive Sludges
Johnston, C. (Author), Tribello, G. (Supervisor) & Kohanoff, J. (Supervisor), Jul 2019
Student thesis: Doctoral Thesis › Doctor of Philosophy

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First principles simulation of cement for nuclear waste disposal
Kavanagh, R. (Author), Kohanoff, J. (Supervisor) & Tribello, G. (Supervisor), Jul 2021
Student thesis: Doctoral Thesis › Doctor of Philosophy

File

Cite this

Le Caër, S., Dezerald, L., Boukari, K., Lainé, M., Taupin, S., Kavanagh, R. M., Johnston, C. S. N., Foy, E., Charpentier, T., Krakowiak, K. J., Pellenq, R. J. M., Ulm, F. J., Tribello, G. A., Kohanoff, J., & Saúl, A. (2017). Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study. Cement and Concrete Research, 100, 110-118. https://doi.org/10.1016/j.cemconres.2017.05.022

@article{1b6874523a884f8d829a9149238a2729,

title = "Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study",

abstract = "Long-term confinement of nuclear waste is one of the main challenges faced by the nuclear industry. Fission products such as 90Sr and 137Cs, both β− emitters known to induce serious health hazards, represent the largest fraction of nuclear waste. Cement is a good candidate to store them, provided it can resist the effects of irradiation over time. Here, we have investigated the effects of β− decay on cement by performing electron irradiation experiments on different samples. We show that H2 production in cement, the main effect of water radiolysis, depends strongly on composition and relative humidity. First-principles calculations indicate that the water-rich interlayer regions with Ca2+ ions act as electron traps that promote the formation of H2. They also show that holes localize in water-rich regions in low Ca content samples and are then able to participate in H2 production. This work provides new understanding of radiolysis effects in cements.",

keywords = "Cement paste, Radiolysis, H2 production, First-principles calculations, Reaction mechanisms",

author = "{Le Ca{\"e}r}, Sophie and Lucile Dezerald and Khaoula Boukari and Maxime Lain{\'e} and S{\'e}bastien Taupin and Kavanagh, {Ryan M.} and Johnston, {Conrad S.N.} and Eddy Foy and Thibault Charpentier and Krakowiak, {Konrad J.} and Pellenq, {Roland J M} and Ulm, {Franz J.} and Tribello, {Gareth A.} and Jorge Kohanoff and Andres Sa{\'u}l",

year = "2017",

month = oct,

doi = "10.1016/j.cemconres.2017.05.022",

language = "English",

volume = "100",

pages = "110--118",

journal = "Cement and Concrete Research",

issn = "0008-8846",

publisher = "Elsevier Ltd",

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Le Caër, S, Dezerald, L, Boukari, K, Lainé, M, Taupin, S, Kavanagh, RM, Johnston, CSN, Foy, E, Charpentier, T, Krakowiak, KJ, Pellenq, RJM, Ulm, FJ, Tribello, GA , Kohanoff, J & Saúl, A 2017, 'Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study', Cement and Concrete Research, vol. 100, pp. 110-118. https://doi.org/10.1016/j.cemconres.2017.05.022

TY - JOUR

T1 - Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study

AU - Le Caër, Sophie

AU - Dezerald, Lucile

AU - Boukari, Khaoula

AU - Lainé, Maxime

AU - Taupin, Sébastien

AU - Kavanagh, Ryan M.

AU - Johnston, Conrad S.N.

AU - Foy, Eddy

AU - Charpentier, Thibault

AU - Krakowiak, Konrad J.

AU - Pellenq, Roland J M

AU - Ulm, Franz J.

AU - Tribello, Gareth A.

AU - Kohanoff, Jorge

AU - Saúl, Andres

PY - 2017/10

Y1 - 2017/10

N2 - Long-term confinement of nuclear waste is one of the main challenges faced by the nuclear industry. Fission products such as 90Sr and 137Cs, both β− emitters known to induce serious health hazards, represent the largest fraction of nuclear waste. Cement is a good candidate to store them, provided it can resist the effects of irradiation over time. Here, we have investigated the effects of β− decay on cement by performing electron irradiation experiments on different samples. We show that H2 production in cement, the main effect of water radiolysis, depends strongly on composition and relative humidity. First-principles calculations indicate that the water-rich interlayer regions with Ca2+ ions act as electron traps that promote the formation of H2. They also show that holes localize in water-rich regions in low Ca content samples and are then able to participate in H2 production. This work provides new understanding of radiolysis effects in cements.

AB - Long-term confinement of nuclear waste is one of the main challenges faced by the nuclear industry. Fission products such as 90Sr and 137Cs, both β− emitters known to induce serious health hazards, represent the largest fraction of nuclear waste. Cement is a good candidate to store them, provided it can resist the effects of irradiation over time. Here, we have investigated the effects of β− decay on cement by performing electron irradiation experiments on different samples. We show that H2 production in cement, the main effect of water radiolysis, depends strongly on composition and relative humidity. First-principles calculations indicate that the water-rich interlayer regions with Ca2+ ions act as electron traps that promote the formation of H2. They also show that holes localize in water-rich regions in low Ca content samples and are then able to participate in H2 production. This work provides new understanding of radiolysis effects in cements.

KW - Cement paste

KW - Radiolysis

KW - H2 production

KW - First-principles calculations

KW - Reaction mechanisms

U2 - 10.1016/j.cemconres.2017.05.022

DO - 10.1016/j.cemconres.2017.05.022

M3 - Article

SN - 0008-8846

VL - 100

SP - 110

EP - 118

JO - Cement and Concrete Research

JF - Cement and Concrete Research

ER -

Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study

Abstract

Keywords

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Student theses

Exploration of Hydrogen Gas Evolution from Radioactive Sludges

First principles simulation of cement for nuclear waste disposal

Cite this