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Two Mechanisms of Slow Host–Guest Complexation between Cucurbit[6]uril and Cyclohexylmethylamine: pH-Responsive Supramolecular Kinetics

✍ Scribed by Cesar Marquez; Werner M. Nau


Publisher
John Wiley and Sons
Year
2001
Tongue
English
Weight
161 KB
Volume
40
Category
Article
ISSN
0044-8249

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✦ Synopsis


20 times more rapid is the complexation of the organic ammonium ion receptor cucurbit[6]uril (CB6) with cyclohexylmethylamine than with the cyclohexylmethylammonium species. Within the narrow pH region around the pK value of the amine, the complexation kinetics are accelerated but the binding constant remains essentially unaffected. In this region, the ammonium complex is formed through binding of the amine form followed by fast protonation and not through direct complexation of the ammonium form. Molecular dynamics calculations suggest that the amine form undergoes a direct inclusion into CB6 while the ingression of the ammonium form is retarded by the formation of an association complex, which reacts through a different, higher lying transition state to the inclusion complex.