The {Pd84}Ac wheel, initially discovered serendipitously, is the only reported giant palladium macrocycle – a unique structure which spontaneously assembles from small building blocks. Efforts to produce analogues of this structure have proved elusive but we have devised a new modular route allowing incorporation of other ligands, and a new screening approach to cluster discovery. We then made structural assignments of new species from solution experiments, overcoming the need for crystallographic analysis. As a result, we were have discovered a family of new palladium macrocycles based on the existing {Pd84}Ac wheel with different ligands and sizes confirming the magic number series for this cluster family. Finally we describe how we were able to produce structures with variable fractions of ‘functional’ ligands. Together these discoveries establish palladium clusters as a new class of tunable nanostructures. In facilitating the discovery of species which would not have been discovered by orthodox crystallization approaches, this work also demonstrates the value of solution-based screening and characterization in cluster chemistry, as a means to decouple cluster formation, discovery, and isolation.

Expansion of the family of gigantic palladium macrocycles based on {Pd84}

253rd National Meeting (2017)

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