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The dimethylchloronium salt [Me2Cl][Al(OTeF5)4] is used to methylate electron‐deficient aromatic systems in Friedel–Crafts type reactions as shown by the synthesis of N‐methylated cations, such as [MeNC5F5]+, [MeNC5F4I]+, and [MeN3C3F3]+. To gain a better understanding of such fundamental Friedel–Crafts reactions, the role of the dimethylchloronium cation has been evaluated by quantum‐chemical calculations. [ABSTRACT FROM AUTHOR]

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A new chloronium‐containing salt, [Me2Cl][Al(OTeF5)4], was synthesized on multigram scale by means of a simple one‐pot procedure. The isolated product can be handled at room temperature and used as a strong electrophilic methylation agent. This is demonstrated by the methylation of the very weak bases P(CF3)3, PF3, MeI, and MeBr. [ABSTRACT FROM AUTHOR]

The pentafluoroorthotellurate (F5TeO–, teflato) group was transferred to two organonickel precursors resulting in the formation of [Ni(Hacac)2(OTeF5)2] and [Ni(iPrIm)2(OTeF5)2]. These complexes show completely different behavior in their stability against stronger coordinating agents, coordination arrangement, and their spin state. Interestingly, traces of water did not hydrolyze the teflato ligand, instead coordinating to the central nickel atom with formation of a dinuclear complex [{Ni(Hacac)(H2O)(OTeF5)(μ‐OTeF5)}2]. [ABSTRACT FROM AUTHOR]