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Photochemical Synthesis and Characterization of a Uranyl Peroxide Triethylamine N‐OxideDimer
Journal article   Open access   Peer reviewed

Photochemical Synthesis and Characterization of a Uranyl Peroxide Triethylamine N‐OxideDimer

Brett Lottes and Korey P. Carter
European journal of inorganic chemistry, Vol.27(28), e202400300
10/01/2024
DOI: 10.1002/ejic.202400300
url
https://doi.org/10.1002/ejic.202400300View
Published (Version of record) Open Access

Abstract

A µ‐peroxido‐bis[di‐triethylamine N‐oxide‐dichloro‐dioxouranium] complex with the formula [(UO2)2O2(ON(CH2CH3)3)4Cl2] (complex 1) was synthesized photochemically from a reaction containing uranyl chloride, triethylamine, and H2O2. The photochemical breakdown of H2O2 yielded •OH radicals that reacted with triethylamine to form triethylamine N‐oxide (TEAO) in situ, which subsequently coordinated to UO22+ cations in a monodentate fashion via the N‐oxide functional groups. Structure determination using single crystal X‐ray diffraction revealed that TEAO ligands also formed intermolecular and intramolecular hydrogen bonds with UO22+ and peroxide moieties, and the intermolecular H‐bonding interactions displayed a temperature dependence with Oyl ‐ ‐ H – C and Oper ‐ ‐ H – C distances shortening at 100(2) K by ca. 0.1 Å. Raman spectroscopy data were collected on single crystals of 1 and peak fitting of these results allowed for assignments of peaks including C‐N stretches for TEAO ligands bound to UO22+ cations at 696.8 cm‐1, 717.8 cm‐1, and 776.5 cm‐1, which are redshifted by approximately 30 cm‐1 when compared to free triethylamine. UO22+ν1 and O22‐ν1 stretches, U‐Oper stretches, and notably, U‐Cl stretches were all identified as well, with U‐Cl modes at 198.9 cm‐1 and 212.1 cm‐1 substantially redshifted compared to the uranyl chloride starting material.
Photochemistry uranium in situ ligand synthesis uranyl peroxide oxygen radicals UIOWA OA Agreement

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