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

Research output: Contribution to journalArticle

3 Citations (Scopus)

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
Pages (from-to)9387-9391
Number of pages5
JournalJournal of the American Chemical Society
Volume140
Issue number30
DOIs
Publication statusPublished - Aug 1 2018

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Paraquat
Electrons
Viologens
Solid state devices
Quantum chemistry
Crystals
X ray crystallography
X Ray Crystallography
Electron Spin Resonance Spectroscopy
Oxidation-Reduction
Paramagnetic resonance
Tuning
Single crystals
Equipment and Supplies

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., ... 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

Mixed-Valence Superstructure Assembled from a Mixed-Valence Host-Guest Complex. / Liu, Zhichang; Frasconi, Marco; Liu, Wei Guang; Zhang, Yu; Dyar, Scott M.; Shen, Dengke; Sarjeant, Amy A.; Goddard, William A.; Wasielewski, Michael R; Stoddart, J. Fraser.

In: Journal of the American Chemical Society, Vol. 140, No. 30, 01.08.2018, p. 9387-9391.

Research output: Contribution to journalArticle

Liu, Z, Frasconi, M, Liu, WG, Zhang, Y, Dyar, SM, Shen, D, Sarjeant, AA, Goddard, WA, Wasielewski, MR & Stoddart, JF 2018, 'Mixed-Valence Superstructure Assembled from a Mixed-Valence Host-Guest Complex', Journal of the American Chemical Society, vol. 140, no. 30, pp. 9387-9391. https://doi.org/10.1021/jacs.8b05322
Liu, Zhichang ; Frasconi, Marco ; Liu, Wei Guang ; Zhang, Yu ; Dyar, Scott M. ; Shen, Dengke ; Sarjeant, Amy A. ; Goddard, William A. ; Wasielewski, Michael R ; Stoddart, J. Fraser. / Mixed-Valence Superstructure Assembled from a Mixed-Valence Host-Guest Complex. In: Journal of the American Chemical Society. 2018 ; Vol. 140, No. 30. pp. 9387-9391.
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