Contribution of the nuclear field shift to kinetic uranium isotope fractionation

Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review

Autoren

  • A. R. Brown
  • Yvonne Röbbert
  • A. Sato
  • M. Hada
  • M. Abe
  • R. Bernier-Latmani

Organisationseinheiten

Externe Organisationen

  • Hiroshima University
  • Eidgenössische Technische Hochschule Lausanne (ETHL)
  • Tokyo Metropolitan University
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Details

OriginalspracheEnglisch
Seiten (von - bis)43-47
Seitenumfang5
FachzeitschriftGeochemical Perspectives Letters
Jahrgang27
Frühes Online-Datum9 Okt. 2023
PublikationsstatusVeröffentlicht - 2023

Abstract

Isotopic fractionation of heavy elements (e.g., >100 amu) often invokes the nuclear field shift effect, which is due to the impact of the elements’ large nuclei on electron density. In particular, it has been explicitly described for uranium (U) at equilibrium and during kinetic isotope fractionation in abiotic mercury reactions. By following the fractionation of 233U, 235U, 236U and 238U during the enzymatic reduction of hexavalent U to tetravalent U by the bacterium Shewanella oneidensis, we provide the first direct evidence of the nuclear field shift effect during biologically controlled kinetic isotope fractionation. Here, we observed the odd-even staggering trend between fractionation factors of each isotope and their nuclear masses, and show that fractionation factors are correlated better with the nuclear volume than the mass. Additionally, by computing the relative contributions of the conventional mass-dependent effect (vibrational energy) and the mass-independent effect (nuclear field shift), we demonstrate that the experimental nuclear field shift effect is smaller than the calculated equilibrium value and that this discrepancy is responsible for the kinetic fractionation factor being lower than that predicted at equilibrium.

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Contribution of the nuclear field shift to kinetic uranium isotope fractionation. / Brown, A. R.; Röbbert, Yvonne; Sato, A. et al.
in: Geochemical Perspectives Letters, Jahrgang 27, 2023, S. 43-47.

Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review

Brown, AR, Röbbert, Y, Sato, A, Hada, M, Abe, M & Bernier-Latmani, R 2023, 'Contribution of the nuclear field shift to kinetic uranium isotope fractionation', Geochemical Perspectives Letters, Jg. 27, S. 43-47. https://doi.org/10.7185/GEOCHEMLET.2333
Brown, A. R., Röbbert, Y., Sato, A., Hada, M., Abe, M., & Bernier-Latmani, R. (2023). Contribution of the nuclear field shift to kinetic uranium isotope fractionation. Geochemical Perspectives Letters, 27, 43-47. https://doi.org/10.7185/GEOCHEMLET.2333
Brown AR, Röbbert Y, Sato A, Hada M, Abe M, Bernier-Latmani R. Contribution of the nuclear field shift to kinetic uranium isotope fractionation. Geochemical Perspectives Letters. 2023;27:43-47. Epub 2023 Okt 9. doi: 10.7185/GEOCHEMLET.2333
Brown, A. R. ; Röbbert, Yvonne ; Sato, A. et al. / Contribution of the nuclear field shift to kinetic uranium isotope fractionation. in: Geochemical Perspectives Letters. 2023 ; Jahrgang 27. S. 43-47.
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AU - Brown, A. R.

AU - Röbbert, Yvonne

AU - Sato, A.

AU - Hada, M.

AU - Abe, M.

AU - Bernier-Latmani, R.

N1 - Publisher Copyright: © 2023 European Association of Geochemistry. All rights reserved.

PY - 2023

Y1 - 2023

N2 - Isotopic fractionation of heavy elements (e.g., >100 amu) often invokes the nuclear field shift effect, which is due to the impact of the elements’ large nuclei on electron density. In particular, it has been explicitly described for uranium (U) at equilibrium and during kinetic isotope fractionation in abiotic mercury reactions. By following the fractionation of 233U, 235U, 236U and 238U during the enzymatic reduction of hexavalent U to tetravalent U by the bacterium Shewanella oneidensis, we provide the first direct evidence of the nuclear field shift effect during biologically controlled kinetic isotope fractionation. Here, we observed the odd-even staggering trend between fractionation factors of each isotope and their nuclear masses, and show that fractionation factors are correlated better with the nuclear volume than the mass. Additionally, by computing the relative contributions of the conventional mass-dependent effect (vibrational energy) and the mass-independent effect (nuclear field shift), we demonstrate that the experimental nuclear field shift effect is smaller than the calculated equilibrium value and that this discrepancy is responsible for the kinetic fractionation factor being lower than that predicted at equilibrium.

AB - Isotopic fractionation of heavy elements (e.g., >100 amu) often invokes the nuclear field shift effect, which is due to the impact of the elements’ large nuclei on electron density. In particular, it has been explicitly described for uranium (U) at equilibrium and during kinetic isotope fractionation in abiotic mercury reactions. By following the fractionation of 233U, 235U, 236U and 238U during the enzymatic reduction of hexavalent U to tetravalent U by the bacterium Shewanella oneidensis, we provide the first direct evidence of the nuclear field shift effect during biologically controlled kinetic isotope fractionation. Here, we observed the odd-even staggering trend between fractionation factors of each isotope and their nuclear masses, and show that fractionation factors are correlated better with the nuclear volume than the mass. Additionally, by computing the relative contributions of the conventional mass-dependent effect (vibrational energy) and the mass-independent effect (nuclear field shift), we demonstrate that the experimental nuclear field shift effect is smaller than the calculated equilibrium value and that this discrepancy is responsible for the kinetic fractionation factor being lower than that predicted at equilibrium.

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JO - Geochemical Perspectives Letters

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