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Tetrathiafulvalene Radical Cation Dimerization in a Bistable Tripodal [4]Rotaxane

✍ Scribed by Ivan Aprahamian; John-Carl Olsen; Ali Trabolsi; J. Fraser Stoddart


Publisher
John Wiley and Sons
Year
2008
Tongue
English
Weight
592 KB
Volume
14
Category
Article
ISSN
0947-6539

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✦ Synopsis


Abstract

The template‐directed synthesis of a bistable tripodal [4]rotaxane, which has cyclobis(paraquat‐p‐phenylene) (CBPQT^4+^) as the π‐electron‐deficient rings, and tetrathiafulvalene (TTF) and 1,5‐dioxynaphthalene units as the pairs of π‐electron‐rich recognition sites located on all three legs of the tripodal dumbbell, is described. The chemical and electrochemical oxidation of the [4]rotaxane and its tripodal dumbbell have allowed us to unravel an unprecedented TTF^.+^ radical cation dimerization. In fact, two types of TTF dimers, namely, the radical cation dimer [TTF^.+^]~2~ and the mixed‐valence one [(TTF)~2~]^.+^, have been observed at room temperature for the tripodal dumbbell, whereas, in the case of the [4]rotaxane, only the radical cation dimer [TTF^.+^]~2~ is formed. This anomaly can be explained if it is accepted that most of the neutral TTF units in the [4]rotaxane are encircled by CBPQT^4+^ rings, which renders the formation of the mixed‐valence dimer [(TTF)~2~]^.+^ highly unfavorable.