A two-dimensional metallosupramolecular framework design based on coordination crosslinking of helical oligoamide nanorods

Norton G. West; Rania S. Seoudi; Anders J. Barlow; Dongchen Qi; Ljiljana Puskar; Mark P. Del Borgo; Ketav Kulkarni; Christopher G. Adda; Jisheng Pan; Marie-Isabel Aguilar; Patrick Perlmutter; Adam Mechler

doi:10.1039/D0MA00123F

A two-dimensional metallosupramolecular framework design based on coordination crosslinking of helical oligoamide nanorods

Norton G. West,†^a Rania S. Seoudi,

†^a Anders J. Barlow,

^a Dongchen Qi,^ab Ljiljana Puskar,

^c Mark P. Del Borgo,^d Ketav Kulkarni,

^d Christopher G. Adda,

^a Jisheng Pan,^e Marie-Isabel Aguilar,^d Patrick Perlmutter^a and Adam Mechler

*^a

Author affiliations

* Corresponding authors

^a Department of Chemistry and Physics, La Trobe Institute for Molecular Science, La Trobe University, Bundoora, Victoria 3086, Australia
E-mail: a.mechler@latrobe.edu.au

^b School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology, Brisbane, Queensland 4001, Australia

^c Monash Biomedicine Discovery Institute & Department of Biochemistry and Molecular Biology, Monash University, Clayton, Victoria 3800, Australia

^d Department Locally Sensitive and Time-Resolved Spectroscopy, Helmholtz-Zentrum Berlin für Materialien und Energie, 12498 Berlin, Germany

^e Institute of Materials Research and Engineering, A*STAR (Agency for Science, Technology and Research), Singapore 138634, Singapore

Abstract

Spontaneous formation of nanostructured materials of defined structure and morphology is a crucial milestone toward realizing true bottom-up nanofabrication. Supramolecular recognition offers unparalleled specificity, selectivity and geometric flexibility to design hierarchical nanostructures. However, competition between similar binding motifs and the dynamic nature of the attachment imposes a severe limitation on the complexity of the achievable structures. Here we outline a design based on two distinct binding motifs in a supramolecular fibrous assembly to realize a metallosupramolecular framework (MSF). Controlled geometries were achieved by one-dimensional supramolecular assembly of substituted oligoamide units. The assembly of the monomers yields nanorods of sub-nanometer diameter and lengths in the 100 μm range. Addition of Cu²⁺ led to the formation of well aligned two-dimensional arrays on mica surface. Vibrational spectroscopy confirmed that the backbone amide moieties are not affected by metal addition. XPS and NEXAFS results suggest that Cu(II) is reduced in the process to a mixture of Cu(I) and Cu(0), likely in an interaction with the amine moiety of the imidazole side chain. Our results indicate that the two dimensional superstructure is based on the formation of polynuclear metal complexes between the oligoamide nanorods, thus the structure is confirmed to be a metallosupramolecular framework.

Materials Advances

A two-dimensional metallosupramolecular framework design based on coordination crosslinking of helical oligoamide nanorods

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A two-dimensional metallosupramolecular framework design based on coordination crosslinking of helical oligoamide nanorods

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