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Molecular Models of Ruthenium(II) Organometallic Complexes  William F. Coleman
The featured molecules for this month come from the paper "Experiments in Thermodynamics and Kinetics of Phosphine Substitution in (p-Cymene)RuCl2(PR3)" by Ozerov, Moura, and Hoffman in which they study the reactions of a number of "piano stool" complexes of ruthenium(II). The synthesis of compound 2a offers students an alternative to the preparation of ferrocene if they are only preparing one metal-arene complex, and the use of the (p-cymene)RuCl2 dimer as a starting material introduces them to a compound that has become important for the synthesis of a number of ruthenium catalysts. Two structures are found for the dimer in the gas phase, one with the chlorides cis to one another and a more stable form with the chlorides trans. DFT calculations using the LanL2MB basis set and the B3LYP functional in Gaussian 03 (1) show the trans form to be about 90 kJ/mol more stable than the cis form. The structures of the trans form of the dimer and of compound 2a are presented in 2 formats with bonds from the ruthenium ion to all of the carbons in the aryl ring and with a single line to a ghost atom in the center of the ring. These are the two common ways of representing such structures but students should be made aware that the overall coordination about the ruthenium in both the dimer and in compound 2a is octahedral, and should look at the structures to convince themselves of that fact. It is also instructive to look at compound 2a, and the other piano stool complexes that are made in the paper, to see how deceptive representation of the triphenylphosphine moiety as PR3 is in terms of the stereochemical bulk of that group.