Abstract
This paper reports on the synthesis and reactivity of Ru(IV) η4-diene complexes of the type Ru(η5-C5Me5)(η4-diene)Br2+ obtained by oxidative bromine additions to Ru(II) η4-diene complexes. Mechanistic details are derived from the reaction products varying with the oxidizing agent and the leaving ligand and are backed up by extended Huckel molecular orbital calculations. The diene fragment in Ru(IV) is prone to gauche deformation and is therefore extremely susceptible to nucleophilic attack of even weak anionic bases generating the corresponding Ru(IV) η3-allyl complexes. Accordingly, Ru(IV) η4-diene complexes are stabilized either by using 2,3-disubstituted diene ligands in which case gauche deformation is highly unfavorable or else by excluding nucleophilic agents. For the latter method, two convenient routes to affording Ru(IV) η4-diene complexes are (i) the reaction of Br+CF3SO3- with Ru(η5-C5Me5)(η4-diene)Br and (ii) the reaction of dibromine with labile Ru(η5-C5Me5)(η4-diene)(CF3SO3). The conversion ...
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