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Single-crystal X-ray diffraction studies revealed that the structures of 1 and 2 consist of a 2-periodic, layer sql motif. This kind of dinuclear ruthenium II arene complex has unique biological characteristics and is a promising model for new anticancer drug development. Highly charged metal ions are difficult to investigate in weakly coordinating ionic liquids ILs because of the insolubility of their solid forms, but the molecular liquid TiCl4 offers a way to react tetravalent metal ions in an IL. Although structurally similar, activated samples of 1 and 2 showed differing gas and vapor sorption capabilities. Cs exchange occurred the fastest and with the greatest capacity when starting in the H-form at room temperature, and at elevated temperatures when starting in the Na-form. To the best of our knowledge, such an abrupt structural transformation by alkaline elements is reported in all-inorganic asymmetric compounds for the first time. Using topological analysis combined with theoretical calculations, the depopulation of dx2—y2 is shown to be due to significant covalency in the Cu—C bonds.

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