Biofunctionalization of Metal–Organic Framework Nanoparticles via Combined Nitroxide-Mediated Polymerization and Nitroxide Exchange Reaction |
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Authors: | Ilona Wagner Simon Spiegel Julian Brückel Matthias Schwotzer Alexander Welle Martina H Stenzel Stefan Bräse Salma Begum Manuel Tsotsalas |
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Affiliation: | 1. Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), Hermann-von Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany;2. Institute for Organic Chemistry (IOC), Karlsruhe Institute of Technology (KIT), Fritz-Haber-Weg 6, 76131 Karlsruhe, Germany;3. Center for Advanced Macromolecular Design, School of Chemistry, University of New South Wales, Sydney, NSW, 2052 Australia |
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Abstract: | Surface engineering of metal–organic framework nanoparticles (MOF NPs), and enabling their post-synthetic modulation that facilitates the formation of bio-interfaces has tremendous potential for diverse applications including therapeutics, imaging, biosensing, and drug-delivery systems. Despite the progress in MOF NPs synthesis, colloidal stability and homogeneous dispersity—a desirable property for biotechnological applications, stands as a critical obstacle and remains a challenging task. In this report, dynamic surfaces modification of MOF NPs with polyethylene glycol (PEG) polymer is described using grafting-from PEGylation by employing nitroxide-mediated polymerization (NMP) and inserting arginylglycylaspartic acid (RGD) peptides on the surface via a nitroxide exchange reaction (NER). The dynamic modification strategy enables tailoring PEG-grafted MOF NPs of the type UiO-66-NH2 with improved colloidal stability, and high dispersity, while the morphology and lattice crystallinity are strictly preserved. The interaction of PEG-grafted MOF NPs with human serum albumin (HSA) protein under physiological conditions is studied. The PEG-grafted colloidal MOF NPs adsorb less HSA protein than the uncoated ones. Therefore, the described approach increases the scope of bio-relevant applications of colloidal MOF NPs by reducing nonspecific interactions using NMP based PEGylation, while preserving the possibility to introduce targeting moieties via NER for specific interactions. |
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Keywords: | MOF nanoparticles nitroxide exchange reaction nitroxide-mediated polymerization post-synthetic modification surface functionalization |
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