期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 133, 期 12, 页码 4538-4547出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja110584c
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资金
- Air Force Office of Scientific Research (AFSOR) [FA9550-07-1-0534]
- National Science Foundation (NSF) [CHE-0924620, CHE-1012378]
- Microelectronics Advanced Research Corporation (MARCO)
- ARO-DURIP
- ONR-DURIP
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-SC0001059, DE-PS-08GO98004P, DE-SC0000989]
- Link Foundation
- International Center for Diffraction Data
- Northwestern University
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1012378, 0924620] Funding Source: National Science Foundation
Two donor-acceptor [3]catenanes-composed of a tetracationic molecular square, cyclobis(paraquat-4,4'-biphenylene), as the pi-electron deficient ring and either two tetrathiafulvalene (TTF) and 1,5-dioxynaphthalene (DNP) containing macrocycles or two TTF-butadiyne-containing macrocycles as the pi-electron rich components have been investigated in order to study their ability to form TTF radical dimers. It has been proven that the mechanically interlocked nature of the [3]catenanes facilitates the formation of the TTF radical dimers under redox control, allowing an investigation to be performed on these intermolecular interactions in a so-called molecular flask under ambient conditions in considerable detail. In addition, it has also been shown that the stability of the TTF radical-cation dimers can be tuned by varying the secondary binding motifs in the [3]catenanes. By replacing the DNP station with a butadiyne group, the distribution of the TTF radical-cation dimer can be changed from 60% to 100%. These findings have been established by several techniques including cyclic voltammetry, spectroelectrochemistry and UV-vis-NIR and EPR spectroscopies, as well as with X-ray diffraction analysis which has provided a range of solid-state crystal structures. The experimental data are also supported by high-level DFT calculations. The results contribute significantly to our fundamental understanding of the interactions within the TTF radical dimers.
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