Joint experimental and theoretical studies of the surprising stability of the aryl pentazole upon noncovalent binding to beta-cyclodextrin
YZ Yang and XF Liu and RB Zhang and SP Pang, PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 19, 31236-31244 (2017).
DOI: 10.1039/c7cp05783k
Herein, binding of the beta-cyclodextrin (beta-CD) host to the unstable aryl pentazole guest has been confirmed experimentally and theoretically. After the confinement of aryl pentazole, electron density reorganization was studied by M06-2X dispersion-corrected DET and further reflected in the characteristic shift in the NMR spectra. Among the host guest complexes, the inclusion complex is favored with the phenyl ring expectedly encapsulated within the cavity through noncovalent interactions such as hydrogen bonding, C-H center dot center dot center dot pi, and the special C-sp2-H center dot center dot center dot H-C-sp3 bonding discovered by the NBO, QTAIM, and NCI-RDG theories. The host guest binding renders the enhancement of the nitrogen-ring aromatic character; this has been analyzed by employing nucleus- independent chemical shift (NICS)-based profiles. The non-covalent interaction largely enhances the thermal stability of the guest through a change of the decomposition reaction path whether the guest is encapsulated or not by the host. By comparison of the structures of B1-B4, the enhancement could be assigned to the ion-type transition structure stabilized by the C-H bonds of the host.
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