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

© 2017 Elsevier Ltd 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 sto...

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Main Authors: Le Caër, Sophie, Dezerald, Lucile, Boukari, Khaoula, Lainé, Maxime, Taupin, Sébastien, Kavanagh, Ryan M, Johnston, Conrad SN, Foy, Eddy, Charpentier, Thibault, Krakowiak, Konrad J, Pellenq, Roland J-M, Ulm, Franz J, Tribello, Gareth A, Kohanoff, Jorge, Saúl, Andres
Format: Article
Language:English
Published: Elsevier BV 2021
Online Access:https://hdl.handle.net/1721.1/135714
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author Le Caër, Sophie
Dezerald, Lucile
Boukari, Khaoula
Lainé, Maxime
Taupin, Sébastien
Kavanagh, Ryan M
Johnston, Conrad SN
Foy, Eddy
Charpentier, Thibault
Krakowiak, Konrad J
Pellenq, Roland J-M
Ulm, Franz J
Tribello, Gareth A
Kohanoff, Jorge
Saúl, Andres
author_facet Le Caër, Sophie
Dezerald, Lucile
Boukari, Khaoula
Lainé, Maxime
Taupin, Sébastien
Kavanagh, Ryan M
Johnston, Conrad SN
Foy, Eddy
Charpentier, Thibault
Krakowiak, Konrad J
Pellenq, Roland J-M
Ulm, Franz J
Tribello, Gareth A
Kohanoff, Jorge
Saúl, Andres
author_sort Le Caër, Sophie
collection MIT
description © 2017 Elsevier Ltd 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.
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spelling mit-1721.1/1357142022-03-31T14:31:26Z Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study Le Caër, Sophie Dezerald, Lucile Boukari, Khaoula Lainé, Maxime Taupin, Sébastien Kavanagh, Ryan M Johnston, Conrad SN Foy, Eddy Charpentier, Thibault Krakowiak, Konrad J Pellenq, Roland J-M Ulm, Franz J Tribello, Gareth A Kohanoff, Jorge Saúl, Andres © 2017 Elsevier Ltd 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. 2021-10-27T20:28:57Z 2021-10-27T20:28:57Z 2017 2019-09-25T15:32:40Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/135714 en 10.1016/J.CEMCONRES.2017.05.022 Cement and Concrete Research Creative Commons Attribution-NonCommercial-NoDerivs License http://creativecommons.org/licenses/by-nc-nd/4.0/ application/pdf Elsevier BV Other repository
spellingShingle Le Caër, Sophie
Dezerald, Lucile
Boukari, Khaoula
Lainé, Maxime
Taupin, Sébastien
Kavanagh, Ryan M
Johnston, Conrad SN
Foy, Eddy
Charpentier, Thibault
Krakowiak, Konrad J
Pellenq, Roland J-M
Ulm, Franz J
Tribello, Gareth A
Kohanoff, Jorge
Saúl, Andres
Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study
title Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study
title_full Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study
title_fullStr Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study
title_full_unstemmed Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study
title_short Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study
title_sort production of h2 by water radiolysis in cement paste under electron irradiation a joint experimental and theoretical study
url https://hdl.handle.net/1721.1/135714
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