Christie, L. G. , Asche, S., Mathieson, J. S., Vila-Nadal, L. and Cronin, L. (2018) Investigating the formation of giant {Pd72}Prop and {Pd84}Gly macrocycles using NMR, HPLC and mass spectrometry. Journal of the American Chemical Society, 140(30), pp. 9379-9382. (doi: 10.1021/jacs.8b05059) (PMID:30005574)
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Abstract
The formation of giant polyoxometalate (POM) species are relatively underexplored as their self-assembly process is complex due to the rapid kinetics. Polyoxopalladates (POPds) are a class of POMs based on Pd, the largest of which is the {Pd84}Ac wheel, and the slower kinetics mean the system is more amenable to systematic study. Here, we show it is possible to follow the assembly of two types of Pd-wheel; the {Pd84}Gly the smaller {Pd72}Prop wheel formed using glycolate and propionate ligands respectively. We analyzed the formation of {Pd72}Prop and {Pd84}Gly using mass spec-trometry (SEC-HPLC-MS and preparative desalting followed by MS). This was accompanied by studies that followed the chemical shift differences between the outer/inner ligands and the free ligand in solution for the {Pd84}Ac, {Pd72}Prop, and {Pd84}Gly species using NMR; this showed it was possible to track the formation of the wheels. Our findings confirm that the macrocycles assemble from smaller building blocks which react together to form the larger species over a period of days. These findings open the way for further structural derivatives and exploration of their host-guest chemistry.
| Item Type: | Articles |
|---|---|
| Status: | Published |
| Refereed: | Yes |
| Glasgow Author(s) Enlighten ID: | Vila-Nadal, Dr Laia and Christie, Miss Lorna and Mathieson, Dr Jennifer and Asche, Silke and Cronin, Professor Lee |
| Authors: | Christie, L. G., Asche, S., Mathieson, J. S., Vila-Nadal, L., and Cronin, L. |
| College/School: | College of Science and Engineering > School of Chemistry |
| Journal Name: | Journal of the American Chemical Society |
| Publisher: | American Chemical Society |
| ISSN: | 0002-7863 |
| ISSN (Online): | 1520-5126 |
| Published Online: | 13 July 2018 |
| Copyright Holders: | Copyright © 2018 American Chemical Society |
| First Published: | First published in Journal of the American Chemical Society 140(30):9379–9382 |
| Publisher Policy: | Reproduced under a Creative Commons License |
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