Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 9, Pages 3371-3377Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b13304
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Funding
- National Science Foundation [CHE-1507321]
- American Chemical Society [56375-ND4]
- Ohio University
- Condensed Matter and Surface Science Program (CMSS) at Ohio University
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1507321] Funding Source: National Science Foundation
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The self-assembly into dynamic oligomers of Cucurbit[8]uril (CB[8]), a positive ditopic Ir(III) bisterpyridine complex, and a negative ditopic Fe(II) bisterpyridine complex flanked by four butyrate side chains was assessed to answer a seemingly straightforward question: does CB [8] adopt a social self-sorting pattern by encapsulating both positive and negative units into a heterotemary complex? We showed that this is indeed the case, with CB[8] linking a positive Ir unit to a neighboring negative Fe unit whenever possible. Furthermore, the solubility of the dynamic oligomers was significantly affected by their sequence; upon addition of 0.6-1.2 equiv of positive Ir oligomer to its negative Fe counterpart, the predominant assembly present in solution was a mixed oligomer with a (Fe-Ir-Ir-)(n) sequence. Weak interactions between the negative butyrate side chains and the partially positive outer wall of CB[7] were also identified by two-dimensional nuclear magnetic resonance techniques, and resulted in a negative pK(a) shift (0.10 pK(a) unit) for the terminal carboxylic groups.
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