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XANES-Based Determination of Redox Potentials Imposed by Steel Corrosion Products in Cement-Based Media

Bin Ma, Alejandro Fernandez-Martinez, Benoît Madé, Nathaniel Findling, Ekaterina Markelova, Eduardo Salas-Colera, Thierry Maffeis Orcid Logo, Aled R. Lewis, Delphine Tisserand, Sarah Bureau, Laurent Charlet

Environmental Science & Technology

Swansea University Author: Thierry Maffeis Orcid Logo

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DOI (Published version): 10.1021/acs.est.8b03236

Abstract

The redox potential (Eh) in a cementitious nuclear waste repository is critical to the retardation behavior of redox-sensitive radionuclides (RNs), and largely controlled by embedded steel corrosion but hard to be determined experimentally. Here, we propose an innovative Eh determination method base...

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Published in: Environmental Science & Technology
ISSN: 0013-936X 1520-5851
Published: 2018
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URI: https://cronfa.swan.ac.uk/Record/cronfa44923
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spelling 2020-06-17T12:08:02.8648380 v2 44923 2018-10-16 XANES-Based Determination of Redox Potentials Imposed by Steel Corrosion Products in Cement-Based Media 992eb4cb18b61c0cd3da6e0215ac787c 0000-0003-2357-0092 Thierry Maffeis Thierry Maffeis true false 2018-10-16 EEEG The redox potential (Eh) in a cementitious nuclear waste repository is critical to the retardation behavior of redox-sensitive radionuclides (RNs), and largely controlled by embedded steel corrosion but hard to be determined experimentally. Here, we propose an innovative Eh determination method based on chemical/spectroscopic measurements. Oxidized nuclides (UVI, SeIV, MoVI, and SbV) were employed as species probes to detect the Eh values imposed by steel (Fe0) and steel corrosion products (magnetite/hematite, and magnetite/goethite couples) in cement pore water. Nuclides showed good sorption affinity, especially toward Fe0, in decreasing Kd order for U &#62; Sb &#62; Se &#62; Mo under both N2 and H2 atmospheres. The reduced nuclide species were identified as UO2, U4O9, FeSe, FeSe2, Se0, Sb0, and Sb2O3, but no redox transformation occurred for Mo. Eh values were obtained by using the Nernst equation. Remarkably, their values fell in a small range centered around −456 mV at pH ∼ 13.5 for both Fe0 and Fe-oxyhydroxides couples. This Eh value appears to be controlled by the nanocrystalline Fe(OH)2/Fe(OH)3 or (Fe1–x,Cax)(OH)2/Fe(OH)3 couple, whose presence was confirmed by pair distribution function analyses. This approach could pave the way for describing the Eh gradient in reinforced concrete where traditional Eh measurements are not feasible. Journal Article Environmental Science & Technology 0013-936X 1520-5851 31 12 2018 2018-12-31 10.1021/acs.est.8b03236 COLLEGE NANME Electronic and Electrical Engineering COLLEGE CODE EEEG Swansea University 2020-06-17T12:08:02.8648380 2018-10-16T16:20:16.1303975 Bin Ma 1 Alejandro Fernandez-Martinez 2 Benoît Madé 3 Nathaniel Findling 4 Ekaterina Markelova 5 Eduardo Salas-Colera 6 Thierry Maffeis 0000-0003-2357-0092 7 Aled R. Lewis 8 Delphine Tisserand 9 Sarah Bureau 10 Laurent Charlet 11 0044923-22102018140619.pdf fernandez-martinez2018.pdf 2018-10-22T14:06:19.6830000 Output 1608488 application/pdf Accepted Manuscript true 2019-09-13T00:00:00.0000000 true eng
title XANES-Based Determination of Redox Potentials Imposed by Steel Corrosion Products in Cement-Based Media
spellingShingle XANES-Based Determination of Redox Potentials Imposed by Steel Corrosion Products in Cement-Based Media
Thierry Maffeis
title_short XANES-Based Determination of Redox Potentials Imposed by Steel Corrosion Products in Cement-Based Media
title_full XANES-Based Determination of Redox Potentials Imposed by Steel Corrosion Products in Cement-Based Media
title_fullStr XANES-Based Determination of Redox Potentials Imposed by Steel Corrosion Products in Cement-Based Media
title_full_unstemmed XANES-Based Determination of Redox Potentials Imposed by Steel Corrosion Products in Cement-Based Media
title_sort XANES-Based Determination of Redox Potentials Imposed by Steel Corrosion Products in Cement-Based Media
author_id_str_mv 992eb4cb18b61c0cd3da6e0215ac787c
author_id_fullname_str_mv 992eb4cb18b61c0cd3da6e0215ac787c_***_Thierry Maffeis
author Thierry Maffeis
author2 Bin Ma
Alejandro Fernandez-Martinez
Benoît Madé
Nathaniel Findling
Ekaterina Markelova
Eduardo Salas-Colera
Thierry Maffeis
Aled R. Lewis
Delphine Tisserand
Sarah Bureau
Laurent Charlet
format Journal article
container_title Environmental Science & Technology
publishDate 2018
institution Swansea University
issn 0013-936X
1520-5851
doi_str_mv 10.1021/acs.est.8b03236
document_store_str 1
active_str 0
description The redox potential (Eh) in a cementitious nuclear waste repository is critical to the retardation behavior of redox-sensitive radionuclides (RNs), and largely controlled by embedded steel corrosion but hard to be determined experimentally. Here, we propose an innovative Eh determination method based on chemical/spectroscopic measurements. Oxidized nuclides (UVI, SeIV, MoVI, and SbV) were employed as species probes to detect the Eh values imposed by steel (Fe0) and steel corrosion products (magnetite/hematite, and magnetite/goethite couples) in cement pore water. Nuclides showed good sorption affinity, especially toward Fe0, in decreasing Kd order for U &#62; Sb &#62; Se &#62; Mo under both N2 and H2 atmospheres. The reduced nuclide species were identified as UO2, U4O9, FeSe, FeSe2, Se0, Sb0, and Sb2O3, but no redox transformation occurred for Mo. Eh values were obtained by using the Nernst equation. Remarkably, their values fell in a small range centered around −456 mV at pH ∼ 13.5 for both Fe0 and Fe-oxyhydroxides couples. This Eh value appears to be controlled by the nanocrystalline Fe(OH)2/Fe(OH)3 or (Fe1–x,Cax)(OH)2/Fe(OH)3 couple, whose presence was confirmed by pair distribution function analyses. This approach could pave the way for describing the Eh gradient in reinforced concrete where traditional Eh measurements are not feasible.
published_date 2018-12-31T03:56:25Z
_version_ 1763752841557573632
score 11.016258

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