Acetate-Induced Disassembly of Spherical Iron Oxide Nanoparticle Clusters into Monodispersed Core−Shell Structures upon Nanoemulsion Fusion

Ahmet Kertmen; Pau Torruella; Emerson Coy; Luis Yate; Grzegorz Nowaczyk; Jacek Gapiński; Carmen Vogt; Muhammet Toprak; Sonia Estrade; Francesca Peiro; Sławomir Milewski; Stefan Jurga; Ryszard Andruszkiewicz

doi:10.1021/acs.langmuir.7b02743

Acetate-Induced Disassembly of Spherical Iron Oxide Nanoparticle Clusters into Monodispersed Core−Shell Structures upon Nanoemulsion Fusion

Abstract

It has been long known that the physical encapsulation of oleic acid-capped iron oxide nanoparticles (OA−IONPs) with the etyltrimethylammonium (CTA+) surfactant induces the formation of spherical iron oxide nanoparticle clusters (IONPCs). However, the behavior and functional properties of IONPCs in chemical reactions have been largely neglected and are still not well-understood. Herein, we report an unconventional ligand-exchange function of IONPCs activated when dispersed in an ethyl acetate/acetate buffer system. The ligand exchange can successfully transform hydrophobic OA−IONP building blocks of IONPCs into highly hydrophilic, acetate-capped iron oxide nanoparticles (Ac−IONPs). More importantly, we demonstrate that the addition of silica precursors (tetraethyl orthosilicate and 3-aminopropyltriethoxysilane) to the acetate/oleate ligand exchange reaction of the IONPs induces the disassembly of the IONPCs into monodispersed iron oxide−acetate−silica core−shell−shell (IONPs@acetate@SiO2) nanoparticles. Our observations evidence that the formation of IONPs@acetate@SiO2 nanoparticles is initiated by a unique micellar fusion mechanism between the Pickering-type emulsions of IONPCs and nanoemulsions of silica precursors formed under ethyl acetate buffered conditions. A dynamic rearrangement of the CTA+−oleate bilayer on the IONPC surfaces is proposed to be responsible for the templating process of the silica shells around the individual IONPs. In comparison to previously reported methods in the literature, our work provides a much more detailed experimental evidence of the silica-coating mechanism in a nanoemulsion system. Overall, ethyl acetate is proven to be a very efficient agent for an effortless preparation of monodispersed IONPs@acetate@SiO2 and hydrophilic Ac−IONPs from IONPCs.

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Authors (13)

Ahmet Kertmen
Pau Torruella
- Universitat de Barcelona Departament d’Electronica
Emerson Coy
- Adam Mickiewicz University NanoBioMedical Centre
Luis Yate
- CIC biomaGUNE, San Sebastian brak
Grzegorz Nowaczyk
- Adam Mickiewicz University NanoBioMedical Centre
Jacek Gapiński
- Adam Mickiewicz University NanoBioMedical Centre
Carmen Vogt
- KTH-Royal Institute of Technology, Stockholm Department of Applied Physics
Muhammet Toprak
- KTH-Royal Institute of Technology, Stockholm Department of Applied Physics
Sonia Estrade
- Universitat de Barcelona Departament d’Electronica
Francesca Peiro
- Universitat de Barcelona Departament d’Electronica
Sławomir Milewski prof. dr hab. inż.
Stefan Jurga prof. dr hab.
- Adam Mickiewicz University NanoBioMedical Centre
Ryszard Andruszkiewicz prof. dr hab. inż.

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Publication version: Accepted or Published Version
DOI:: Digital Object Identifier (open in new tab) 10.1021/acs.langmuir.7b02743
License: Copyright (2017 American Chemical Society)

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Category:: Articles
Type:: artykuł w czasopiśmie wyróżnionym w JCR
Published in:: LANGMUIR no. 33, pages 10351 - 10365,
ISSN: 0743-7463
Language:: English
Publication year:: 2017
Bibliographic description:: Kertmen A., Torruella, P., Coy E., Yate L., Nowaczyk G., Gapiński J., Vogt, C., Toprak M., Estrade S., Peiro F., Milewski S., Jurga S., Andruszkiewicz R.: Acetate-Induced Disassembly of Spherical Iron Oxide Nanoparticle Clusters into Monodispersed Core−Shell Structures upon Nanoemulsion Fusion// LANGMUIR. -Vol. 33, (2017), s.10351-10365
DOI:: Digital Object Identifier (open in new tab) 10.1021/acs.langmuir.7b02743
Verified by:: Gdańsk University of Technology