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Multifunctional Nanoparticles by Coordinative Self-Assembly of His-Tagged Units with Metal–Organic Frameworks

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Pharmaceutical Biotechnology, Department of Pharmacy and Center for NanoScience (CeNS), LMU Munich, 81377 Munich, Germany
Department of Physics and Center for NanoScience (CeNS), LMU Munich, 80539 Munich, Germany
§ Department of Chemistry and Center for NanoScience (CeNS), LMU Munich, 81377 Munich, Germany
Cite this: J. Am. Chem. Soc. 2017, 139, 6, 2359–2368
Publication Date (Web):January 11, 2017
https://doi.org/10.1021/jacs.6b11934
Copyright © 2017 American Chemical Society

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    Abstract

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    Self-assembly of individual units into multicomponent complexes is a powerful approach for the generation of functional superstructures. We present the coordinative interaction of oligohistidine-tags (His-tags) with metal–organic framework nanoparticles (MOF NPs). By this novel concept, different molecular units can be anchored on the outer surface of MOF NPs in a self-assembly process generating multifunctional nanosystems. The article focuses on two main objectives: first, the detailed investigation of the assembly process and fundamental establishment of the novel functionalization concept; and second, its subsequent use for the development of biomacromolecule (e.g., peptides and proteins) delivery vehicles. Three exemplary MOF structures, MIL-88A, HKUST-1, and Zr-fum, based on different metal components, were selected for the external binding of various His-tagged synthetic peptides and recombinant or chemically H6-modified proteins. Evidence for simultaneous assembly of different functional units with Zr-fum MOF NPs as well as their successful transport into living cells illustrate the promising potential of the self-assembly approach for the generation of multifunctional NPs and future biological applications. Taking the high number of possible MOF NPs and different functional units into account, the reported functionalization approach opens great flexibility for the targeted synthesis of multifunctional NPs for specific purposes.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.6b11934.

    • Additional materials and methods, synthesis and analysis of peptides and His-tagged functional units, characterization of MOF NPs (PDF)

    • Movie demonstrating the binding of H6-A647N to HKUST-1 MOF NPs visualized by decoloration of the supernatant after centrifugation (AVI)

    • Three-dimensional reconstruction movie of a HeLa cell treated with Zr-fum/H6-GFP (AVI)

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