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Covalent Post-assembly Modification Triggers Multiple Structural Transformations of a Tetrazine-Edged Fe4L6 Tetrahedron

Roberts, Derrick A.; Pilgrim, Ben S.; Sirvinskaite, Giedre; Ronson, Tanya K.; Nitschke, Jonathan R.

Covalent Post-assembly Modification Triggers Multiple Structural Transformations of a Tetrazine-Edged Fe4L6 Tetrahedron Thumbnail


Authors

Derrick A. Roberts

Giedre Sirvinskaite

Tanya K. Ronson

Jonathan R. Nitschke



Abstract

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 FeII4L6 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.

Citation

Roberts, D. A., Pilgrim, B. S., Sirvinskaite, G., Ronson, T. K., & Nitschke, J. R. (2018). Covalent Post-assembly Modification Triggers Multiple Structural Transformations of a Tetrazine-Edged Fe4L6 Tetrahedron. Journal of the American Chemical Society, 140(30), 9616-9623. https://doi.org/10.1021/jacs.8b05082

Journal Article Type Article
Acceptance Date Jul 7, 2018
Online Publication Date Jul 8, 2018
Publication Date 2018-08
Deposit Date Feb 24, 2020
Publicly Available Date Apr 21, 2020
Journal Journal of the American Chemical Society
Print ISSN 0002-7863
Electronic ISSN 1520-5126
Publisher American Chemical Society
Peer Reviewed Peer Reviewed
Volume 140
Issue 30
Pages 9616-9623
DOI https://doi.org/10.1021/jacs.8b05082
Keywords Supramolecular Chemistry; Organic Chemistry; Self-Assembly; Metal-Organic Cages
Public URL https://nottingham-repository.worktribe.com/output/4026108
Publisher URL https://pubs.acs.org/doi/10.1021/jacs.8b05082
Additional Information This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/jacs.8b05082.

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