Reactions of actinide ions with ethylene oxide

Journal of Mass Spectrometry : JMS
John K Gibson

Abstract

Naked and oxo-ligated actinide (An) monopositive ions were reacted with ethylene oxide, cyclo-C(2)H(4)O (EtO). Along with An = U, Np, Pu and Am, ions of two lanthanide (Ln) elements, Ln = Tb and Tm, were studied for comparison. Metal and metal oxide ions, M(+), MO(+) and MO(2)(+), were generated by laser ablation and immediately reacted with EtO. Unreacted and product ions were detected by time-of-flight mass spectrometry. It was apparent that the overall reaction cross-sections decreased in the order U(+) > or = Np(+) > Pu(+) > Am(+). A primary reaction channel for each studied metal was the formation of MO(+) from M(+), in accord with the expected exothermicity of oxygen abstraction from EtO. For U, Np and Pu, the dioxides were also major products, indicating OAn(+)--O dissociation energies of at least 350 kJ mol(-1), the energy required for O-atom abstraction from EtO. For Am, Tb and Tm, the dioxides were only very minor products, reflecting the stabilities of the trivalent states and resistance to oxidation to higher valence states; the structures/bonding in these MO(2)(+) are intriguing given that the formal pentavalent bonding state is effectively unattainable. It was demonstrated that EtO, unlike more thermochemically fa...Continue Reading

References

Nov 5, 1999·Journal of Mass Spectrometry : JMS·J K Gibson
Apr 24, 1996·Inorganic Chemistry·Christoph HeinemannHelmut Schwarz

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Citations

Nov 5, 2003·Journal of the American Society for Mass Spectrometry·Michael Van StipdonkDorothy Hanna
Aug 15, 2014·The Journal of Physical Chemistry. a·Michael J Van StipdonkJohn K Gibson
Jul 9, 2016·Rapid Communications in Mass Spectrometry : RCM·Michael J Van StipdonkTheodore A Corcovilos
Jun 8, 2001·Journal of Mass Spectrometry : JMS
Jan 20, 2006·The Journal of Physical Chemistry. a·Michael J Van StipdonkGary S Groenewold
Apr 6, 2006·Journal of the American Chemical Society·Gary S GroenewoldLucas Visscher

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