Guest Exchange through Facilitated Transport in a Seemingly Impenetrable Hydrogen-Bonded Framework

Yuantao Li, Marcel Handke, Yu Sheng Chen, Alexander G. Shtukenberg, Chunhua T. Hu, Michael Ward

Research output: Contribution to journalArticle

Abstract

A new inclusion compound consisting of a guanidinium 1,3,5-tri(4-sulfophenyl)benzene (G3TSPHB) host framework containing isophorone guests that surround isolated and seemingly inaccessible pockets was amenable to guest exchange with hexafluorobenzene (HFB) through a single crystal-single crystal transformation (SCSCT). Single-crystal X-ray diffraction of intermediate transformation states, from the parent compound G3TSPHB·(isophorone)3.7·(methanol)5.4 to the final state G3TSPHB·(isophorone)3.1·(HFB)2·(methanol)2, indicated a crystal symmetry change from monoclinic to hexagonal prior to full incorporation of HFB. Optical microscopy during the SCSCT revealed the formation of lamellae, which expanded and then coalesced into a single crystal when the phase transformation was complete. In situ Raman microscopy revealed changes in the orientation of isophorone guests during the transformation that suggested a pathway for HFB entry into the host cavities. The SCSCT occurs more rapidly than expected on the basis of simple diffusion, consistent with facilitated transport along the lamellae interfaces and a reduction in the length scale for guest exchange.

Original languageEnglish (US)
Pages (from-to)12915-12921
Number of pages7
JournalJournal of the American Chemical Society
Volume140
Issue number40
DOIs
StatePublished - Oct 10 2018

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Hydrogen
Guanidine
Benzene
Single crystals
Methanol
Microscopy
X-Ray Diffraction
hexafluorobenzene
isophorone
Crystal symmetry
Optical microscopy
Ion exchange
Microscopic examination
Phase transitions
X ray diffraction

ASJC Scopus subject areas

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

Cite this

Guest Exchange through Facilitated Transport in a Seemingly Impenetrable Hydrogen-Bonded Framework. / Li, Yuantao; Handke, Marcel; Chen, Yu Sheng; Shtukenberg, Alexander G.; Hu, Chunhua T.; Ward, Michael.

In: Journal of the American Chemical Society, Vol. 140, No. 40, 10.10.2018, p. 12915-12921.

Research output: Contribution to journalArticle

Li, Yuantao ; Handke, Marcel ; Chen, Yu Sheng ; Shtukenberg, Alexander G. ; Hu, Chunhua T. ; Ward, Michael. / Guest Exchange through Facilitated Transport in a Seemingly Impenetrable Hydrogen-Bonded Framework. In: Journal of the American Chemical Society. 2018 ; Vol. 140, No. 40. pp. 12915-12921.
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