Overcoming the crystallization bottleneck: a family of gigantic inorganic {Pdx}L(x=84, 72) palladium macrocycles discovered using solution techniques

Christie, L. G. , Surman, A. J. , Scullion, R. A., Xu, F., Long, D.-L. and Cronin, L. (2016) Overcoming the crystallization bottleneck: a family of gigantic inorganic {Pdx}L(x=84, 72) palladium macrocycles discovered using solution techniques. Angewandte Chemie (International Edition), 55(41), pp. 12741-12745. (doi:10.1002/anie.201606005) (PMID:27634480) (PMCID:PMC5113701)

[img]
Preview
Text
128887.pdf - Published Version
Available under License Creative Commons Attribution.

2MB

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.

Item Type:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Long, Dr De Liang and Cronin, Professor Leroy and Christie, Miss Lorna and Surman, Dr Andrew
Authors: Christie, L. G., Surman, A. J., Scullion, R. A., Xu, F., Long, D.-L., and Cronin, L.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Angewandte Chemie (International Edition)
Publisher:Wiley
ISSN:1433-7851
ISSN (Online):1521-3773
Published Online:16 September 2016
Copyright Holders:Copyright © 2016 The Authors
First Published:First published in Angewandte Chemie (International Edition) 55(41):12741-12745
Publisher Policy:Reproduced under a Creative Commons License

University Staff: Request a correction | Enlighten Editors: Update this record

Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
577391Programmable Molecular Metal Oxides (PMMOs) - From Fundamentals to ApplicationLeroy CroninEngineering & Physical Sciences Research Council (EPSRC)EP/J015156/1CHEM - CHEMISTRY
646611Programmable 'Digital' Synthesis for Discovery and Scale-up of Molecules, Clusters and NanomaterialsLeroy CroninEngineering & Physical Sciences Research Council (EPSRC)EP/L023652/1CHEM - CHEMISTRY
562821Innovative Manufacturing Research Centre for Continuous Manufacturing and Crystallisation (CMAC)Leroy CroninEngineering & Physical Sciences Research Council (EPSRC)EP/I033459/1CHEM - CHEMISTRY
616021Energy and the Physical Sciences: Hydrogen Production using a Proton Electron BufferLeroy CroninEngineering & Physical Sciences Research Council (EPSRC)EP/K023004/1CHEM - CHEMISTRY
599451Microscale Chemically Reactive Electronic AgentsLeroy CroninEuropean Commission (EC)FP7 ICT MICRE31CHEM - CHEMISTRY