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A Comparative IRMPD and DFT Study of Fe 3+ and UO 2 2+ Complexation with N -Methylacetohydroxamic Acid

Abstract : Iron(III) and uranyl complexes of N-methylacetohydroxamic acid (NMAH) have been investigated by mass spectrometry, infrared multiphoton dissociation (IRMPD) spectroscopy, and density functional theory (DFT) calculations. A comparison between IRMPD and theoretical IR spectra enabled one to probe the structures for some selected complexes detected in the gas phase. The results show that coordination of Fe3+ and UO22+ by hydroxamic acid is of a very similar nature. Natural bond orbital analysis suggests that bonding in uranyl complexes possesses a slightly stronger ionic character than that in iron complexes. Collision-induced dissociation (CID), IRMPD, and O-18-labeling experiments unambiguously revealed a rare example of the U=O bond activation concomitant with the elimination of a water molecule from the gaseous [UO2(NMA)(NMAH)(2)](+) complex. The U=O bond activation is observed only for complexes with one monodentate NMAH molecule forming a hydrogen bond toward one "yl" oxygen atom, as was found by DFT calculations. This reactivity might explain oxygen exchange observed for uranyl complexes.
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Soumis le : lundi 20 décembre 2021 - 15:24:34
Dernière modification le : vendredi 14 octobre 2022 - 04:06:26


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Thibault Terencio, Jana Roithová, Stéphane Brandès, Yoann Rousselin, Marie-José Penouilh, et al.. A Comparative IRMPD and DFT Study of Fe 3+ and UO 2 2+ Complexation with N -Methylacetohydroxamic Acid. Inorganic Chemistry, 2018, 57 (3), pp.1125 - 1135. ⟨10.1021/acs.inorgchem.7b02567⟩. ⟨hal-01857041⟩



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