Mixed-Valence Superstructure Assembled from a Mixed-Valence Host-Guest Complex

Zhichang Liu*, Marco Frasconi, Wei Guang Liu, Yu Zhang, Scott M. Dyar, Dengke Shen, Amy A. Sarjeant, William A. Goddard, Michael R. Wasielewski, J. Fraser Stoddart

*Corresponding author for this work

Research output: Contribution to journalArticle

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Abstract

Herein, we report an unprecedented mixed-valence crystal superstructure that consists of a 2:1 host-guest complex [MV⊂(CBPQT)2]2/3+ [MV = methyl viologen, CBPQT = cyclobis(paraquat-p-phenylene)]. One electron is distributed statistically between three [MV⊂(CBPQT)2]•+ composed of a total of 15 viologen units. The mixed-valence state is validated by single-crystal X-ray crystallography, which supports an empirical formula of [MV⊂(CBPQT)2]3·(PF6)2 for the body-centered cubic superstructure. Electron paramagnetic resonance provides further evidence of electron delocalization. Quantum chemistry calculations confirm the mixed-valence state in the crystal superstructure. Our findings demonstrate that precise tuning of the redox states in host-guest systems can lead to a promising supramolecular strategy for achieving long-range electron delocalization in solid-state devices.

Original languageEnglish (US)
Pages (from-to)9387-9391
Number of pages5
JournalJournal of the American Chemical Society
Volume140
Issue number30
DOIs
StatePublished - Aug 1 2018

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ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Liu, Z., Frasconi, M., Liu, W. G., Zhang, Y., Dyar, S. M., Shen, D., Sarjeant, A. A., Goddard, W. A., Wasielewski, M. R., & Stoddart, J. F. (2018). Mixed-Valence Superstructure Assembled from a Mixed-Valence Host-Guest Complex. Journal of the American Chemical Society, 140(30), 9387-9391. https://doi.org/10.1021/jacs.8b05322