Synthesis of a Hexachloro Sulfate(IV) Dianion Enabled by Polychloride Chemistry

多氯化物化学促进六氯硫酸(IV)二阴离子的合成

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Abstract

The preparation and structural characterization of [NEt(3) Me](2) [SCl(6) ] is described, which is the first example of a [SCl(6) ](2-) dianion and of a halosulfate anion of the type [S(x) X(y) ](z-) in general. This dianion belongs to the group of 14-valence electron AB(6) E systems and forms an octahedral structure in the solid-state. Interestingly, co-crystallization with CH(2) Cl(2) affords [NEt(3) Me](2) [SCl(6) ]⋅4 CH(2) Cl(2) containing [SCl(6) ](2-) dianions with C(4v) symmetry. As suggested by quantum-chemical calculations, the distortion of the structure is not caused by a stereochemically active lone pair but by enhanced hydrogen bonding interactions with CH(2) Cl(2) . At elevated temperatures, [NEt(3) Me](2) [SCl(6) ] decomposes to various sulfur chlorine compounds as shown by Raman spectroscopy. Cooling back to room temperature results in the selective formation of [NEt(3) Me](2) [SCl(6) ] which is comparable to the well-studied SCl(4) .

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