Pentavalent U Reactivity Impacts U Isotopic Fractionation during Reduction by Magnetite

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Autoren

  • Zezhen Pan
  • Luca Loreggian
  • Yvonne Roebbert
  • Barbora Bartova
  • Myrtille O.J.Y. Hunault
  • Stefan Weyer
  • Rizlan Bernier-Latmani

Externe Organisationen

  • Fudan University
  • Eidgenössische Technische Hochschule Lausanne (ETHL)
  • Synchrotron SOLEIL
Forschungs-netzwerk anzeigen

Details

OriginalspracheEnglisch
Seiten (von - bis)6595-6604
Seitenumfang10
FachzeitschriftEnvironmental Science and Technology
Jahrgang58
Ausgabenummer15
Frühes Online-Datum4 Apr. 2024
PublikationsstatusVeröffentlicht - 16 Apr. 2024

Abstract

Meaningful interpretation of U isotope measurements relies on unraveling the impact of reduction mechanisms on the isotopic fractionation. Here, the isotope fractionation of hexavalent U [U(VI)] was investigated during its reductive mineralization by magnetite to intermediate pentavalent U [U(V)] and ultimately tetravalent U [U(IV)]. As the reaction proceeded, the remaining aqueous phase U [containing U(VI) and U(V)] systematically carried light isotopes, whereas in the bicarbonate-extracted solution [containing U(VI) and U(V)], the δ238U values varied, especially when C/C0 approached 0. This variation was interpreted as reflecting the variable relative contribution of unreduced U(VI) (δ238U < 0‰) and bicarbonate-extractable U(V) (δ238U > 0‰). The solid remaining after bicarbonate extraction included unextractable U(V) and U(IV), for which the δ238U values consistently followed the same trend that started at 0.3-0.5‰ and decreased to ∼0‰. The impact of PIPES buffer on isotopic fractionation was attributed to the variable abundance of U(V) in the aqueous phase. A few extremely heavy bicarbonate-extracted δ238U values were due to mass-dependent fractionation resulting from several hypothesized mechanisms. The results suggest the preferential accumulation of the heavy isotope in the reduced species and the significant influence of U(V) on the overall isotopic fractionation, providing insight into the U isotope fractionation behavior during its abiotic reduction process.

ASJC Scopus Sachgebiete

Zitieren

Pentavalent U Reactivity Impacts U Isotopic Fractionation during Reduction by Magnetite. / Pan, Zezhen; Loreggian, Luca; Roebbert, Yvonne et al.
in: Environmental Science and Technology, Jahrgang 58, Nr. 15, 16.04.2024, S. 6595-6604.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Pan, Z, Loreggian, L, Roebbert, Y, Bartova, B, Hunault, MOJY, Weyer, S & Bernier-Latmani, R 2024, 'Pentavalent U Reactivity Impacts U Isotopic Fractionation during Reduction by Magnetite', Environmental Science and Technology, Jg. 58, Nr. 15, S. 6595-6604. https://doi.org/10.1021/acs.est.3c10324
Pan, Z., Loreggian, L., Roebbert, Y., Bartova, B., Hunault, M. O. J. Y., Weyer, S., & Bernier-Latmani, R. (2024). Pentavalent U Reactivity Impacts U Isotopic Fractionation during Reduction by Magnetite. Environmental Science and Technology, 58(15), 6595-6604. https://doi.org/10.1021/acs.est.3c10324
Pan Z, Loreggian L, Roebbert Y, Bartova B, Hunault MOJY, Weyer S et al. Pentavalent U Reactivity Impacts U Isotopic Fractionation during Reduction by Magnetite. Environmental Science and Technology. 2024 Apr 16;58(15):6595-6604. Epub 2024 Apr 4. doi: 10.1021/acs.est.3c10324
Pan, Zezhen ; Loreggian, Luca ; Roebbert, Yvonne et al. / Pentavalent U Reactivity Impacts U Isotopic Fractionation during Reduction by Magnetite. in: Environmental Science and Technology. 2024 ; Jahrgang 58, Nr. 15. S. 6595-6604.
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title = "Pentavalent U Reactivity Impacts U Isotopic Fractionation during Reduction by Magnetite",
abstract = "Meaningful interpretation of U isotope measurements relies on unraveling the impact of reduction mechanisms on the isotopic fractionation. Here, the isotope fractionation of hexavalent U [U(VI)] was investigated during its reductive mineralization by magnetite to intermediate pentavalent U [U(V)] and ultimately tetravalent U [U(IV)]. As the reaction proceeded, the remaining aqueous phase U [containing U(VI) and U(V)] systematically carried light isotopes, whereas in the bicarbonate-extracted solution [containing U(VI) and U(V)], the δ238U values varied, especially when C/C0 approached 0. This variation was interpreted as reflecting the variable relative contribution of unreduced U(VI) (δ238U < 0‰) and bicarbonate-extractable U(V) (δ238U > 0‰). The solid remaining after bicarbonate extraction included unextractable U(V) and U(IV), for which the δ238U values consistently followed the same trend that started at 0.3-0.5‰ and decreased to ∼0‰. The impact of PIPES buffer on isotopic fractionation was attributed to the variable abundance of U(V) in the aqueous phase. A few extremely heavy bicarbonate-extracted δ238U values were due to mass-dependent fractionation resulting from several hypothesized mechanisms. The results suggest the preferential accumulation of the heavy isotope in the reduced species and the significant influence of U(V) on the overall isotopic fractionation, providing insight into the U isotope fractionation behavior during its abiotic reduction process.",
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author = "Zezhen Pan and Luca Loreggian and Yvonne Roebbert and Barbora Bartova and Hunault, {Myrtille O.J.Y.} and Stefan Weyer and Rizlan Bernier-Latmani",
note = "Funding Information: The work at Fudan received supports from the National Natural Science Foundation of China (42107228) and the Shanghai Pujiang Program (21PJ1401000), and the work at EPFL was supported by Swiss National Science Foundation Grant 200021E-164209 and European Research Council Consolidator Grant 725675 (UNEARTH). ",
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volume = "58",
pages = "6595--6604",
journal = "Environmental Science and Technology",
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TY - JOUR

T1 - Pentavalent U Reactivity Impacts U Isotopic Fractionation during Reduction by Magnetite

AU - Pan, Zezhen

AU - Loreggian, Luca

AU - Roebbert, Yvonne

AU - Bartova, Barbora

AU - Hunault, Myrtille O.J.Y.

AU - Weyer, Stefan

AU - Bernier-Latmani, Rizlan

N1 - Funding Information: The work at Fudan received supports from the National Natural Science Foundation of China (42107228) and the Shanghai Pujiang Program (21PJ1401000), and the work at EPFL was supported by Swiss National Science Foundation Grant 200021E-164209 and European Research Council Consolidator Grant 725675 (UNEARTH).

PY - 2024/4/16

Y1 - 2024/4/16

N2 - Meaningful interpretation of U isotope measurements relies on unraveling the impact of reduction mechanisms on the isotopic fractionation. Here, the isotope fractionation of hexavalent U [U(VI)] was investigated during its reductive mineralization by magnetite to intermediate pentavalent U [U(V)] and ultimately tetravalent U [U(IV)]. As the reaction proceeded, the remaining aqueous phase U [containing U(VI) and U(V)] systematically carried light isotopes, whereas in the bicarbonate-extracted solution [containing U(VI) and U(V)], the δ238U values varied, especially when C/C0 approached 0. This variation was interpreted as reflecting the variable relative contribution of unreduced U(VI) (δ238U < 0‰) and bicarbonate-extractable U(V) (δ238U > 0‰). The solid remaining after bicarbonate extraction included unextractable U(V) and U(IV), for which the δ238U values consistently followed the same trend that started at 0.3-0.5‰ and decreased to ∼0‰. The impact of PIPES buffer on isotopic fractionation was attributed to the variable abundance of U(V) in the aqueous phase. A few extremely heavy bicarbonate-extracted δ238U values were due to mass-dependent fractionation resulting from several hypothesized mechanisms. The results suggest the preferential accumulation of the heavy isotope in the reduced species and the significant influence of U(V) on the overall isotopic fractionation, providing insight into the U isotope fractionation behavior during its abiotic reduction process.

AB - Meaningful interpretation of U isotope measurements relies on unraveling the impact of reduction mechanisms on the isotopic fractionation. Here, the isotope fractionation of hexavalent U [U(VI)] was investigated during its reductive mineralization by magnetite to intermediate pentavalent U [U(V)] and ultimately tetravalent U [U(IV)]. As the reaction proceeded, the remaining aqueous phase U [containing U(VI) and U(V)] systematically carried light isotopes, whereas in the bicarbonate-extracted solution [containing U(VI) and U(V)], the δ238U values varied, especially when C/C0 approached 0. This variation was interpreted as reflecting the variable relative contribution of unreduced U(VI) (δ238U < 0‰) and bicarbonate-extractable U(V) (δ238U > 0‰). The solid remaining after bicarbonate extraction included unextractable U(V) and U(IV), for which the δ238U values consistently followed the same trend that started at 0.3-0.5‰ and decreased to ∼0‰. The impact of PIPES buffer on isotopic fractionation was attributed to the variable abundance of U(V) in the aqueous phase. A few extremely heavy bicarbonate-extracted δ238U values were due to mass-dependent fractionation resulting from several hypothesized mechanisms. The results suggest the preferential accumulation of the heavy isotope in the reduced species and the significant influence of U(V) on the overall isotopic fractionation, providing insight into the U isotope fractionation behavior during its abiotic reduction process.

KW - isotope fractionation

KW - pentavalent uranium

KW - redox tracer

KW - uranium remediation

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DO - 10.1021/acs.est.3c10324

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VL - 58

SP - 6595

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JO - Environmental Science and Technology

JF - Environmental Science and Technology

SN - 0013-936X

IS - 15

ER -

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