Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 30, Pages 9616-9623Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b05082
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Funding
- Royal Commission for the Exhibition of 1851 Fellowship
- UK Engineering and Physical Sciences Research Council [EP/M01083X/1]
- Diamond Light Source (UK) [MT11397]
- EPSRC [EP/M01083X/1] Funding Source: UKRI
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Covalent post-assembly modification (PAM) reactions are useful synthetic tools for functionalizing and stabilizing self-assembled metal-organic complexes. Recently, PAM reactions have also been explored as stimuli for triggering supramolecular structural transformations. Herein we demonstrate the use of inverse electron-demand Diels-Alder (IEDDA) PAM reactions to induce supramolecular structural transformations starting from a tetrazine-edged (Fe4L6)-L-II tetrahedral precursor. Following PAM, this tetrahedron rearranged to form three different architectures depending on the addition of other stimuli: an electron-rich aniline or a templating anion. By tracing the stimulus-response relationships within the system, we deciphered a network of transformations that mapped different combinations of stimuli onto specific transformation products. Given the many functions being developed for self-assembled three-dimensional architectures, this newly established ability to control the interconversion between structures using combinations of different stimulus types may serve as the basis for switching the functions expressed within a system.
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