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• W2952892775 abstract "The salt, [F4S═NXe][AsF6], has been synthesized by the solid-state rearrangement of [F3S≡NXeF][AsF6] and by HF-catalyzed rearrangement of [F3S≡NXeF][AsF6] in anhydrous HF (aHF) and HF/BrF5 solvents. The F4S═NXe+ cation undergoes HF solvolysis to form F4S═NH2+, XeF2, and the recently reported F5SN(H)Xe+ cation. Both [F4S═NXe][AsF6] and [F4S═NH2][AsF6] have been characterized by 129Xe and 19F NMR spectroscopy in aHF and HF/BrF5 solvents and by single-crystal X-ray diffraction. The [F4S═NXe][AsF6] salt was also characterized by Raman spectroscopy. The Xe−N bond of F4S═NXe+ is among the shortest Xe−N bonds presently known (2.084(3) Å), and the cation interacts with the AsF6− anion by means of a Xe---F—As bridge in which the Xe---F distance (2.618(2) Å) is significantly less than the sum of the Xe and F van der Waals radii. Both F4S═NXe+ and F4S═NH2+ exhibit trigonal bipyramidal geometries about sulfur, with nitrogen in the equatorial plane and the nitrogen substituents coplanar with the axial fluorine ligands of sulfur. The F4S═NH2+ cation is isoelectronic with F4S═CH2 and, like F4S═CH2, has a high barrier to rotation about the S═N double bond and to pseudorotation of the trigonal bipyramidal F4S═N− moiety. The solution and solid-state rearrangements of F3S≡NXeF+ to F4S═NXe+ are proposed to result from attack at sulfur by fluoride ion arising from HF in solution and from the AsF6− anion in the solid state. Quantum-chemical calculations were employed to calculate the gas-phase geometries, charges, bond orders, valencies, and vibrational frequencies of F4S═NXe+ and F4S═NH2+. The F4S═NXe+ cation provides the first example of xenon bonded to an imido-nitrogen, and together with the F4S═NH2+ cation are presently the only cations known to contain the F4S═N-group. Both cations are intermediates in the HF solvolysis pathways of F3S≡NXeF+ which lead to F5SN(H)Xe+ and F5SNH3+, and significantly extend the chemistry of the F4S═N-group." @default.
• W2952892775 created "2019-06-27" @default.
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• W2952892775 date "2009-05-11" @default.
• W2952892775 modified "2023-10-18" @default.
• W2952892775 title "Solid-State and Solution Rearrangements of F₃S≡NXeF⁺ Leading to the F₄S═NXe⁺ Cation; Syntheses, HF Solvolyses, and Structural Characterizations of [F₄S═NXe][AsF₆] and [F₄S═NH₂][AsF₆]" @default.
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• W2952892775 doi "https://doi.org/10.1021/ja901187n" @default.
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