Oxidation of gas-phase protactinium ions, Pa+ and Pa2+: formation and properties of PaO2(2+)(g), protactinyl

The Journal of Physical Chemistry. a
Marta SantosRussell M Pitzer

Abstract

Oxidation reactions of bare and ligated, monopositive, and dipositive Pa ions in the gas phase were studied by Fourier transform ion cyclotron resonance mass spectrometry. Seven oxidants were employed, ranging from the thermodynamically robust N(2)O to the relatively weak CH(2)O-all oxidized Pa(+) to PaO(+) and PaO(+) to PaO(2)(+). On the basis of experimental observations, it was established that D[Pa(+)-O] and D[OPa(+)-O] > or = 751 kJ mol(-1). Estimates for D[Pa(+)-O], D[OPa(+)-O], IE[PaO], and IE[PaO(2)] were also obtained. The seven oxidants reacted with Pa(2+) to produce PaO(2+), indicating that D[Pa(2+)-O] > or = 751 kJ mol(-1). A particularly notable finding was the oxidation of PaO(2+) by N(2)O to PaO(2)(2+), a species, which formally comprises Pa(VI). Collision-induced dissociation of PaO(2)(2+) suggested the protactinyl connectivity, {O-Pa-O}(2+). The experimentally determined IE[PaO(2)(+)] approximately 16.6 eV is in agreement with self-consistent-field and configuration interaction calculations for PaO(2)(+) and PaO(2)(2+). These calculations provide insights into the electronic structures of these ions and indicate the participation of 5f orbitals in bonding and a partial "6p hole" in the case of protactinyl. It w...Continue Reading

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Citations

Jan 10, 2012·Journal of Mass Spectrometry : JMS·Daniel RiosMichael J Van Stipdonk
Nov 18, 2008·The Journal of Physical Chemistry. a·Joaquim MarçaloRichard G Haire
Oct 17, 2008·The Journal of Physical Chemistry. a·John K GibsonJoaquim Marçalo
Sep 10, 2009·The Journal of Physical Chemistry. a·K Balasubramanian, Zhiji Cao
Nov 6, 2009·The Journal of Physical Chemistry. a·Isaiah Shavitt
Nov 29, 2012·The Journal of Physical Chemistry. a·Célia LourençoMaria Conceição Oliveira
Mar 14, 2012·The Journal of Physical Chemistry. a·Marta SantosMaria Conceição Oliveira
Feb 14, 2015·Chemical Reviews·Attila KovácsLaura Gagliardi

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