Abstract | The 62-CVE clusters Ru₄(µ-RC₂R)₂(CO)₁₁, which feature a dodecahedral cluster core, are readily reduced to a 64-CVE dianion in a process that is essentially chemically reversible. A combination of electrochemical, spectroelectrochemical, and computational analyses of the system indicates that the first formed dianion, which features a square planar arrangement of the metal centers with the alkyne ligands located on opposite faces of the M₄ square and oriented in a manner such that the C-C bonds are perpendicular to each other, undergoes a thermal rearrangement giving a product in which the alkyne vectors lie parallel to each other across the metal framework. |
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