Particle Engineering via Supramolecular Assembly of Macroscopic Hydrophobic Building Blocks

Author:

Kim Chan‐Jin1ORCID,Goudeli Eirini1ORCID,Ercole Francesca2,Ju Yi13ORCID,Gu Yuang1ORCID,Xu Wanjun1ORCID,Quinn John F.24ORCID,Caruso Frank1ORCID

Affiliation:

1. Department of Chemical Engineering The University of Melbourne Parkville Victoria 3010 Australia

2. Drug Delivery Disposition and Dynamics Theme Monash Institute of Pharmaceutical Sciences Monash University Parkville Victoria 3052 Australia

3. School of Science RMIT University Melbourne Victoria 3000 Australia

4. Department of Chemical Engineering Faculty of Engineering Monash University Clayton Victoria 3800 Australia

Abstract

AbstractTailoring the hydrophobicity of supramolecular assembly building blocks enables the fabrication of well‐defined functional materials. However, the selection of building blocks used in the assembly of metal–phenolic networks (MPNs), an emerging supramolecular assembly platform for particle engineering, has been essentially limited to hydrophilic molecules. Herein, we synthesized and applied biscatechol‐functionalized hydrophobic polymers (poly(methyl acrylate) (PMA) and poly(butyl acrylate) (PBA)) as building blocks to engineer MPN particle systems (particles and capsules). Our method allowed control over the shell thickness (e.g., between 10 and 21 nm), stiffness (e.g., from 10 to 126 mN m−1), and permeability (e.g., 28–72 % capsules were permeable to 500 kDa fluorescein isothiocyanate‐dextran) of the MPN capsules by selection of the hydrophobic polymer building blocks (PMA or PBA) and by controlling the polymer concentration in the MPN assembly solution (0.25–2.0 mM) without additional/engineered assembly processes. Molecular dynamics simulations provided insights into the structural states of the hydrophobic building blocks during assembly and mechanism of film formation. Furthermore, the hydrophobic MPNs facilitated the preparation of fluorescent‐labeled and bioactive capsules through postfunctionalization and also particle–cell association engineering by controlling the hydrophobicity of the building blocks. Engineering MPN particle systems via building block hydrophobicity is expected to expand their use.

Funder

Australian Research Council

National Health and Medical Research Council

Publisher

Wiley

Subject

General Chemistry,Catalysis

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