Mineralogical reactions in the Tournemire argillite after in-situ interaction with steels

Gaudin, A.; Gaboreau, Stéphane; Tinseau, E.; Bartier, Danièle; Petit, Sabine; Grauby, Olivier; Foct, F.; Beaufort, Daniel

doi:10.1016/j.clay.2008.08.007

Cited by 38 publications

(11 citation statements)

References 23 publications

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“…Until now, most of the experimental studies related to nuclear waste disposal have focused on iron-clay interaction (Guillaume, 2002;Perronnet, 2004;De Combarieu et al, 2007;Martin et al, 2008;Gaudin et al, 2009) and iron corrosion rate (Reardon, 1995(Reardon, , 2005Féron et al, 2008) to sustain previously mentioned models.…”

Section: Introductionmentioning

confidence: 97%

Kinetics of pyrite to pyrrhotite reduction by hydrogen in calcite buffered solutions between 90 and 180°C: Implications for nuclear waste disposal

Truche

Berger

Destrigneville

et al. 2010

Geochimica et Cosmochimica Acta

112

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Section: Introductionmentioning

confidence: 97%

Kinetics of pyrite to pyrrhotite reduction by hydrogen in calcite buffered solutions between 90 and 180°C: Implications for nuclear waste disposal

Truche

Berger

Destrigneville

et al. 2010

Geochimica et Cosmochimica Acta

112

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“…Such experiments were conducted over timescales varying from years to decades. According to the experiments dismantled and studied so far, much less smectite alteration has been noted under such conditions (compared to controlled small-scale experiments), but magnetite, Fe (oxyhydr)oxides, and siderite were observed as corrosion products (Papillon et al 2003;Carlson et al 2007;Martin et al 2008;Gaudin et al 2009;Schlegel et al 2010;Wersin et al 2015). Despite the numerous investigations, the overall mechanisms of interaction between corroding steel and bentonite are still to be defined (Kaufhold et al 2015).…”

Section: Introductionmentioning

confidence: 99%

Eighteen years of steel–bentonite interaction in the FEBEX in situ test at the Grimsel Test Site in Switzerland

Hadi

Wersin

Serneels

et al. 2019

Clays and clay miner.

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Corrosion of steel canisters containing buried high-level radioactive waste is a relevant issue for the long-term integrity of repositories. The purpose of the present study was to evaluate this issue by examining two differently corroded blocks originating from a full-scale in situ test of the FEBEX bentonite site in Switzerland. The FEBEX experiment was designed initially as a feasibility test of an engineered clay barrier system and was recently dismantled after 18 years of activity. Samples were studied by Fspatially resolved`and Fbulk`experimental methods, including Scanning Electron Microscopy, Elemental Energy Dispersive Spectroscopy (SEM-EDX), μ-Raman spectroscopy, X-ray Fluorescence (XRF), X-ray Diffraction (XRD), and 57 Fe Mössbauer spectrometry, with a focus on Fe-bearing phases. In one of the blocks, corrosion of the steel liner led to diffusion of Fe into the bentonite, resulting in the formation of large (width > 140 mm) red, orange, and blue colored halos. Goethite was identified as the main corrosion product in the red and orange zones while no excess Fe 2+ (compared to the unaffected bentonite) was observed there. Excess Fe 2+ was found to have diffused further into the clay (in the blue zones) but its speciation could not be unambiguously clarified. The results indicate the occurrence of newly formed octahedral Fe 2+ either as Fe 2+ sorbed on the clay or as structural Fe 2+ inside the clay (following electron transfer from sorbed Fe 2+). No other indications of clay transformation or newly formed clay phases were found. The overall pattern indicates that diffusion of Fe was initiated when oxidizing conditions were still prevailing inside the bentonite block, resulting in the accumulation of Fe 3+ close to the interface (up to three times the original Fe content), and continued when reducing conditions were reached, allowing deeper diffusion of Fe 2+ into the clay (inducing an increase of 10-12% of the Fe content).

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“…Ces phases se sont formées par la précipitation d'ions sulfures (S 2− ) avec les ions ferreux (Fe 2+ ) relargués dans le milieu suite aux processus de corrosion du fer métal. Les ions sulfures du milieu sont issus dans le cas de cette expérience soit de l'activité bactérienne [13,37,38], soit de la dissolution de la pyrite contenue dans l'argilite [39][40][41]. En conditions anoxiques, la pyrite est peu soluble [42,43] ce qui rend l'origine biotique des sulfures de fer plus probables.…”

Section: Discussionunclassified

Détermination de la bio-origine des sulfures de fer présents dans les systèmes de corrosion anoxiques par analyse de la composition isotopique du soufre en nanoSIMS

Grousset

Mostefaoui

Chautard

et al. 2016

Matériaux & Techniques

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Résumé -Cetteétude est consacréeà la détermination de l'origine biotique ou abiotique de sulfures de fer formés au cours de processus de corrosion anoxiques par l'analyse de la composition isotopique du soufre. Usuellement ces analyses sont réalisées par IRMS (Isotopic Ratio Mass Spectrometry) sur des sulfures et des sulfates préalablement dissous. Dans cetteétude, en revanche, une nouvelle approche est utilisée, basée sur des analyses isotopiques locales de surface réalisées en nanoSIMS afin de conserver l'information sur la localisation des produits de corrosion. Deux types d'échantillons ontétéétudiés : unéchantillon (CBCC) corrodé pendant 13 mois en conditions contrôlées, et unéchantillon archéologique corrodé pendant environ 2000 ans dans des conditions mal connues. Lorsque le système de corrosion est parfaitement connu, tel que le cas de l'échantillon CBCC, l'analyse isotopique locale par nanoSIMS permet effectivement de conclure sur la (bio-)origine des liserés de sulfures de fer formés. En revanche, lorsque la composition isotopique de la source de sulfates est inconnue, comme dans le cas de l'échantillon archéologique, il n'est pas toujours possible de conclure sur l'origine des sulfures de fer observés. Mots clés : Corrosion anoxique / sulfures de fer / bactéries / fractionnement isotopique du soufre / nanoSIMSAbstract -Characterisation and determination of the bio-origin of iron sulphides in anoxic corrosion systems thanks to isotopic analyses by nanoSIMS. This study is devoted to the determination of the bacterial or inorganic origin of iron sulphides formed during anoxic corrosion processes by sulfur isotopic composition analyses. Broadly, these analyses are realized by IRMS on dissolved sulphides and sulphates. Yet in this study, surface local isotopic analyses are realized by nanoSIMS in order to preserve the information about the corrosion products' localization. Two kinds of samples are studied: a sample (CBCC) corroded during 13 months in controlled laboratory conditions; and one archeological sample corroded during about 2000 years in not very well known conditions. When the corrosion system is perfectly well known, as for the CBCC sample, the local isotopic analyses by nanoSIMS actually enable to conclude on the (bio-)origin of the iron sulphides observed. However, when the isotopic composition of the sulphate's source is unknown, as for the archeological sample, the origin of iron sulphides cannot always be determined.

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Mineralogical reactions in the Tournemire argillite after in-situ interaction with steels

Cited by 38 publications

References 23 publications

Kinetics of pyrite to pyrrhotite reduction by hydrogen in calcite buffered solutions between 90 and 180°C: Implications for nuclear waste disposal

Kinetics of pyrite to pyrrhotite reduction by hydrogen in calcite buffered solutions between 90 and 180°C: Implications for nuclear waste disposal

Eighteen years of steel–bentonite interaction in the FEBEX in situ test at the Grimsel Test Site in Switzerland

Détermination de la bio-origine des sulfures de fer présents dans les systèmes de corrosion anoxiques par analyse de la composition isotopique du soufre en nanoSIMS

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