Fractionnement isotopique

Résumé

Un fractionnement isotopique est une différence de comportement entre différents isotopes d'un même élément chimique lors d'un processus physique ou chimique donné, si bien que le ou les rapports isotopiques varient au cours du processus. C'est notamment le cas lors d'un changement d'état inabouti, d'une réaction chimique partielle ou d'un écoulement à travers un milieu poreux : le produit de la transformation partielle a une composition isotopique légèrement différente de celle du matériau de départ. La différence est plus notable pour les éléments légers (de faible masse atomique) que pour les éléments plus lourds. Quand on considère plus de deux isotopes, la variation des différentes propriétés quantitatives entre ces isotopes est pratiquement proportionnelle à leur différence de masse. En pratique on désigne souvent par « fractionnement isotopique » (voire simplement « fractionnement ») le rapport de fractionnement \alpha=r_\text{arrivée}/r_\text{départ} (où r

Source officielle

https://fr.wikipedia.org/wiki/Fractionnement_isotopique

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Understanding process and role of biomineralization (minerals formed by living organisms) in context of Earth's evolution,global chemical cycles, climatic changes and remediation.

Le cours "Microbiologie pour l'ingénieur" couvre les processus microbiens principaux qui ont lieu dans l'environnement et dans des systèmes de traitement. Il présente les cycles des éléments qui sont catalysés par des microorganismes et qui ont un impact important sur la planète Terre.

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Uranium Isotope Fractionation during the Anoxic Mobilization of Noncrystalline U(IV) by Ligand Complexation

Rizlan Bernier-Latmani, Ashley Richards Brown

Uranium (U) isotopes are suggested as a tool to trace U reduction. However, noncrystalline U(IV), formed predominantly in near-surface environments, may be complexed and remobilized using ligands under anoxic conditions. This may cause additional U isotope fractionation and alter the signatures generated by U reduction. Here, we investigate the efficacy of noncrystalline U(IV) mobilization by ligand complexation and the associated U isotope fractionation. Noncrystalline U(IV) was produced via the reduction of U(VI) (400 μM) by Shewanella oneidensis MR-1 and was subsequently mobilized with EDTA (1 mM), citrate (1 mM), or bicarbonate (500 mM) in batch experiments. Complexation with all investigated ligands resulted in significant mobilization of U(IV) and led to an enrichment of 238U in the mobilized fraction (δ238U = 0.4–0.7 ‰ for EDTA; 0.3 ‰ for citrate; 0.2–0.3 ‰ for bicarbonate). For mobilization with bicarbonate, a Rayleigh approach was the most suitable isotope fractionation model, yielding a fractionation factor α of 1.00026–1.00036. Mobilization with EDTA could be modeled with equilibrium isotope fractionation (α: 1.00039–1.00049). The results show that U isotope fractionation associated with U(IV) mobilization under anoxic conditions is significant and needs to be considered when applying U isotopes in remediation monitoring or as a paleo-redox proxy.

2021

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Uranium isotopic signatures can be harnessed to monitor the reductive remediation of subsurface contamination or to reconstruct paleo-redox environments. However, the mechanistic underpinnings of the isotope fractionation associated with U reduction remain poorly understood. Here, we present a coprecipitation study, in which hexavalent U (U(VI)) was reduced during the synthesis of magnetite and pentavalent U (U(V)) was the dominant species. The measured δ238U values for unreduced U(VI) (∼−1.0‰), incorporated U (96 2% U(V), ∼−0.1‰), and extracted surface U (mostly U(IV), ∼0.3‰) suggested the preferential accumulation of the heavy isotope in reduced species. Upon exposure of the U-magnetite coprecipitate to air, U(V) was partially reoxidized to U(VI) with no significant change in the δ238U value. In contrast, anoxic amendment of a heavy isotope-doped U(VI) solution resulted in an increase in the δ238U of the incorporated U species over time, suggesting an exchange between incorporated and surface/aqueous U. Overall, the results support the presence of persistent U(V) with a light isotope signature and suggest that the mineral dynamics of iron oxides may allow overprinting of the isotopic signature of incorporated U species. This work furthers the understanding of the isotope fractionation of U associated with iron oxides in both modern and paleo-environments.

2022

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Mechanism of uranium reduction and immobilization in Desulfovibrio vulgaris biofilms

Rizlan Bernier-Latmani, Malgorzata Alicja Stylo

The prevalent formation of noncrystalline U(IV) species in the subsurface and their enhanced susceptibility to reoxidation and remobilization, as compared to crystalline uraninite, raise concerns about the long-term sustainability of the bioremediation of U-contaminated sites. The main goal of this study was to resolve the remaining uncertainty concerning the formation mechanism of noncrystalline U(IV) in the environment. Controlled laboratory biofilm systems (biotic, abiotic, and mixed biotic abiotic) were probed using a combination of U isotope fractionation and X-ray absorption spectroscopy (XAS). Regardless of the mechanism of U reduction, the presence of a biofilm resulted in the formation of noncrystalline U(IV). Our results also show that biotic U reduction is the most effective way to immobilize and reduce U. However, the mixed biotic abiotic system resembled more closely an abiotic system: (i) the U(IV) solid phase lacked a typically biotic isotope signature and (ii) elemental sulfur was detected, which indicates the oxidation of sulfide coupled to U(VI) reduction. The predominance of abiotic U reduction in our systems is due to the lack of available aqueous U(VI) species for direct enzymatic reduction. In contrast, in cases where bicarbonate is present at a higher concentration, aqueous U(VI) species dominate, allowing biotic U reduction to outcompete the abiotic processes.

Amer Chemical Soc2015

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