Abstract: | On the Structure of Two Isothiazolium Polyiodides (C19H16FeNS)I5 and (C15H12NS)2I8 By oxidation of 3‐phenylamino thiopropenones with iodine two isothiazolium polyiodides were obtained, whose structures have been determined by X‐ray structure analysis. 2‐Phenyl‐5‐ferrocenyl‐isothiazolium pentaiodide(C19H16FeNS)I5 forms a layer structure with isothiazolium cations and polyiodide anions. The polyiodide layers contain pentaiodide ions I5–, triiodide ions I3– and iodine molecules I2. Bis(2,5‐diphenyl‐isothiazolium) octaiodide (C15H12NS)2I8 also forms a layer structure with isothiazolium cations and polyiodide anions. The polyiodide layers are built up by octaiodide ions I82–, pentaiodide ions I5– and triiodide ions I3–. |