A preliminary investigation into the feasibility of using organozirconium reagents to functionalize the methyl groups of polydimethylsiloxanes is made. Hexamethyldisiloxane is deprotonated and then bound to Zr to give CpaZrtCHaSiMeaOSiMesla (1) and Cp*ZrCl2(CH2-SiMe2OSiMe3) (3). These represent the first well-characterized compounds possessing methylsiloxane coordinated to zirconium. X-ray crystallography of 1 and 3 reveals a monodentate and a bidentate coordination mode, respectively, with 3 possessing an unexpected and very weak bond to the siloxane oxygen [Zr-0 = 2.427 (3) Á]. This is among the longest Zr-0 bonds known. Data for 1: cell constants a = 8.330
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