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Overcoming the Crystallization Bottleneck: A Family of Gigantic Inorganic {Pd x } L ( x= 84, 72) Palladium Macrocycles Discovered using Solution Techniques

DOI: 10.1002/ange.201606005 DOI Help

Authors: Lorna G. Christie (WEST Chem, School of Chemistry, University of Glasgow) , Andrew J. Surman (WEST Chem, School of Chemistry, University of Glasgow) , Rachel A. Scullion (WEST Chem, School of Chemistry, University of Glasgow) , Feng Xu (WEST Chem, School of Chemistry, University of Glasgow) , De-liang Long (WEST Chem, School of Chemistry, University of Glasgow) , Leroy Cronin (WEST Chem, School of Chemistry, University of Glasgow)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Angewandte Chemie , VOL 128 , PAGES 12933 - 12937

State: Published (Approved)
Published: October 2016
Diamond Proposal Number(s): 14652

Open Access Open Access

Abstract: The {Pd84}Ac wheel, initially discovered serendipitously, is the only reported giant palladium macrocycle—a unique structure that spontaneously assembles from small building blocks. Analogues of this structure are elusive. A new modular route to {Pd84}Ac is described, allowing incorporation of other ligands, and a new screening approach to cluster discovery. Structural assignments were made of new species from solution experiments, overcoming the need for crystallographic analysis. As a result, two new palladium macrocycles were discovered: a structural analogue of the existing {Pd84}Ac wheel with glycolate ligands, {Pd84}Gly, and the next in a magic number series for this cluster family—a new {Pd72}Prop wheel decorated with propionate ligands. These findings confirm predictions of a magic number rule for the family of {Pdx} macrocycles. Furthermore, structures with variable fractions of functional ligands were obtained. Together these discoveries establish palladium clusters as a new class of tunable nanostructures. In facilitating the discovery of species that 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.

Journal Keywords: Größenausschluss; Ionenbeweglichkeit; Palladium; Polyoxopalladate; Selbstorganisation

Subject Areas: Materials, Chemistry


Instruments: I19-Small Molecule Single Crystal Diffraction

Added On: 18/11/2016 15:09

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Christie_et_al-2016-Angewandte_Chemie.pdf

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