Heterometallic Uranyl (Hydroxyethyl)iminodiacetic Acid (Heidi) Complexes: Molecular Models for U(VI) Uptake in Complex Media

Abstract

AbstractAmidoximated absorbents (AO‐PAN) effectively remove U(VI) from aqueous solution, but previous studies reported more variability for complex natural waters that contain additional confounding ions and molecules. Ternary phases containing U(VI), M(III) (M=Fe(III), Al(III), Ga(III)), and organic molecules exist under these conditions and cause heterogeneous U(VI) uptake on AO‐PAN. The goal of the current study is to provide additional insights into the structural features ternary complexes using N‐(2‐hydroxyethyl)‐iminodiacetic acid (HEIDI) as the model organic chelator and explore the relevance of these species on U(VI) capture. Three model compounds ([(UO2)(Fe)2(μ3‐O)(C6NO5H8)2(H2O)4] (UFe2), ([(UO2)(Al)2(μ2‐OH)(C6NO5H8)2(H2O)3] (UAl2) and [(UO2)(Ga)2(μ2‐OH)(C6NO5H8)2(H2O)3] (UGa2)) were characterized by single‐crystal X‐ray diffraction. Raman spectra of the model compounds were compared with solution data and the ternary phases were noted in the case of Al(III) and Ga(III), but not in the Fe(III) system. U(VI) adsorption onto AO‐PAN was not impacted by the presence of HEIDI or the trivalent metal species.