Bambusuril as a One-Electron Donor for Photoinduced Electron Transfer to Methyl Viologen in Mixed Crystals

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Authors

FIALA Tomáš LUDVÍKOVÁ Lucie HEGER Dominik ŠVEC Jan SLANINA Tomáš VETRÁKOVÁ Ľubica BABIAK Michal NEČAS Marek KULHÁNEK Petr KLÁN Petr ŠINDELÁŘ Vladimír

Year of publication 2017
Type Article in Periodical
MU Faculty or unit

Faculty of Science

Citation
Web http://pubs.acs.org/doi/10.1021/jacs.6b08589
Doi http://dx.doi.org/10.1021/jacs.6b08589
Field Organic chemistry
Keywords DENSITY-FUNCTIONAL CALCULATIONS; ORDER REGULAR APPROXIMATION; CHARGE-TRANSFER SALTS; MOLECULAR-DYNAMICS; CATION RADICALS; METHYLVIOLOGEN; REDUCTION; PHOTOCHEMISTRY; ORGANOSILICA; ACETONITRILE
Description Methyl viologen hexafluorophosphate (MV2+center dot 2PF(6)(-)) and dodecamethylbambus[6]uril (BU6) form crystals in which the layers of viologen dications alternate with those of a 1:2 supramolecular complex of BU6 and PF6-. This arrangement allows for a one-electron reduction of MV2+ ions upon UV irradiation to form MV+center dot radical cations within the crystal structure with half-lives of several hours in air. The mechanism of this photoinduced electron transfer in the solid state and the origin of the long-lived charge-separated state were studied by steady-state and transient spectroscopies, cyclic voltammetry, and electron paramagnetic resonance spectroscopy. Our experiments are supported by quantum-chemical calculations showing that BU6 acts as a reductant. In addition, analogous photochemical behavior is also demonstrated on other MV2+/BU6 crystals containing either BF4- or Br- counterions.
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