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Binding of anions in triply interlocked coordination catenanes and dynamic allostery for dehalogenation reactions

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Abstract

By synergistic combination of multicomponent self-assembly and template-directed approaches, triply interlocked metal organic catenanes that consist of two isolated chirally identical tetrahedrons were constructed and stabilized as thermodynamic minima. In the presence of suitable template anions, the structural conversion from the isolated tetrahedral conformers into locked catenanes occurred via the cleavage of an intrinsically reversible coordination bond in each of the tetrahedrons, followed by the reengineering and interlocking of two fragments with the regeneration of the broken coordination bonds. The presence of several kinds of individual pocket that were attributed to the triply interlocked patterns enabled the possibility of encapsulating different anions, allowing the dynamic allostery between the unlocked/locked conformers to promote the dehalogenation reaction of 3-bromo-cyclohexene efficiently, as with the use of dehalogenase enzymes. The interlocked structures could be unlocked into two individual tetrahedrons through removal of the well-matched anion templates. The stability and reversibility of the locked/unlocked structures were further confirmed by the catching/releasing process that accompanied emission switching, providing opportunities for the system to be a dynamic molecular logic system.

Graphical abstract: Binding of anions in triply interlocked coordination catenanes and dynamic allostery for dehalogenation reactions

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Publication details

The article was received on 17 Sep 2017, accepted on 30 Nov 2017 and first published on 30 Nov 2017


Article type: Edge Article
DOI: 10.1039/C7SC04070A
Citation: Chem. Sci., 2018, Advance Article
  • Open access: Creative Commons BY-NC license
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    Binding of anions in triply interlocked coordination catenanes and dynamic allostery for dehalogenation reactions

    L. Yang, X. Jing, B. An, C. He, Y. Yang and C. Duan, Chem. Sci., 2018, Advance Article , DOI: 10.1039/C7SC04070A

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