4 years ago

Conformational Selection as the Mechanism of Guest Binding in a Flexible Supramolecular Host

Conformational Selection as the Mechanism of Guest Binding in a Flexible Supramolecular Host
F. Dean Toste, Kenneth N. Raymond, Cynthia M. Hong, Robert G. Bergman, David M. Kaphan
This study offers a detailed mechanistic investigation of host–guest encapsulation behavior in a new enzyme–mimetic metal–ligand host and provides the first observation of a conformational selection mechanism (as opposed to induced fit) in a supramolecular system. The Ga4L4 host described features a C3-symmetric ligand motif with meta-substituted phenyl spacers, which enables the host to initially self-assemble into an S4-symmetric structure and then subsequently isomerize to a T-symmetric tetrahedron for better accommodation of a sufficiently large guest. Selective inversion recovery 1H NMR studies provide structural insights into the self-exchange behaviors of the host and the guest individually in this dynamic system. Kinetic analysis of the encapsulation–isomerization event revealed that increasing the concentration of guest inhibits the rate of host–guest relaxation, a key distinguishing feature of conformational selection. A comprehensive study of this simple enzyme mimic provides insight into analogous behavior in biophysics and enzymology and aims to inform the design of efficient self-assembled microenvironment catalysts.

Publisher URL: http://dx.doi.org/10.1021/jacs.7b03812

DOI: 10.1021/jacs.7b03812

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