Investigating the Formation of Giant {Pd72 }Prop and {Pd84 }Gly Macrocycles Using NMR, HPLC, and Mass Spectrometry

Journal of the American Chemical Society
Lorna G ChristieLeroy Cronin

Abstract

The formation of giant polyoxometalate (POM) species is 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 its slower kinetics mean the system is more amenable to systematic study. Here, we show that it is possible to follow the assembly of two types of Pd wheels, {Pd84}Gly and the smaller {Pd72}Prop, formed using glycolate and propionate ligands, respectively. We analyzed the formation of {Pd72}Prop and {Pd84}Gly using mass spectrometry (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, which showed it was possible to track the formation of the wheels. Our findings confirm that the macrocycles assemble from smaller building blocks that 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.

References

Mar 18, 2009·Journal of the American Chemical Society·Ayala ZivIra A Weinstock
Feb 5, 2010·Angewandte Chemie·De-Liang LongLeroy Cronin
Aug 27, 2011·Physical Chemistry Chemical Physics : PCCP·Laia Vilà-NadalJosep M Poblet
Jul 4, 2012·Proceedings of the National Academy of Sciences of the United States of America·Feng XuLeroy Cronin
Aug 22, 2012·Angewandte Chemie·Natalya V IzarovaUlrich Kortz
Apr 15, 2015·Journal of the American Chemical Society·Nancy WatfaEmmanuel Cadot
Aug 1, 2015·Chemistry : a European Journal·Thanh-Loan LaiEmmanuel Cadot
Dec 5, 2017·Journal of the American Chemical Society·Xiu-Ying ZhengLan-Sun Zheng

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Citations

Aug 15, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Xing-Xing ShiMing-Hua Zeng
Oct 30, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Kai-Qiang MoFu-Pei Liang
May 24, 2019·Journal of the American Chemical Society·Fangyuan SongGreta R Patzke

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