Surprises in the Solvent-Induced Self-Ionization in the Uranium Tetrahalide UX4(X = Cl, Br, I)/Ethyl Acetate System

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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä

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en

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9

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ACS Omega, Volume 7, issue 14, pp. 11995–12003

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The reaction of the uranium(IV) halides UCl4, UBr4, or UI4 with ethyl acetate (EtOAc) leads to the formation of the complexes [UX3(EtOAc)4][UX5(EtOAc)] (X = Cl, Br) or [UI4(EtOAc)3]. Thus, both UCl4 and UBr4 show self-ionization in ethyl acetate to a distorted pentagonal bipyramidal [UX3(EtOAc)4]+ cation and a distorted octahedral [UX5(EtOAc)]- anion. Surprisingly, the chloride and bromide compounds are not isotypic. While [UCl3(EtOAc)4][UCl5(EtOAc)] crystallizes in the orthorhombic crystal system, space group P212121 at 250 K, the bromide compound crystallizes in the monoclinic crystal system, P121/n1 at 100 K. Unexpectedly, UI4 does not show self-ionization but forms [UI4(EtOAc)3] molecules, which crystallize in the monoclinic crystal system, P21/c, at 100 K. The compounds were characterized by single-crystal X-ray diffraction, IR, Raman, and NMR spectroscopy, as well as molecular quantum chemical calculations using solvent models.

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Funding Information: We thank the Deutsche Forschungsgemeinschaft for funding. T.G. thanks the HPC-EUROPA3 (INFRAIA-2016-1-730897) for a travel grant and the computing resources provided by CSC, the Finnish IT Center for Science. Publisher Copyright: © 2022 American Chemical Society. All rights reserved.

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Deubner, H L, Graubner, T, Buchner, M R, Weigend, F, Ivlev, S I, Karttunen, A J & Kraus, F 2022, 'Surprises in the Solvent-Induced Self-Ionization in the Uranium Tetrahalide UX 4 (X = Cl, Br, I)/Ethyl Acetate System', ACS Omega, vol. 7, no. 14, pp. 11995–12003. https://doi.org/10.1021/acsomega.2c00175