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Structure Tuning of Electrostatically Self-Assembled Nanoparticles through pH

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Department of Chemistry and Pharmacy and Interdisciplinary Center for Molecular Materials (ICMM), Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstraße 3, D-91058 Erlangen, Germany
Institut Laue-Langevin, DS/LSS, 71 Avenue des Martyrs, F-38000 Grenoble, France
Cite this: J. Phys. Chem. B 2016, 120, 7, 1380–1389
Publication Date (Web):December 3, 2015
https://doi.org/10.1021/acs.jpcb.5b10966
Copyright © 2015 American Chemical Society

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    Abstract

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    pH can be used to tune the self-assembly of cationic polyelectrolyte dendrimers and oppositely charged dyes and to produce particles with a desired shape and size in aqueous solution. We present fundamental insight into the effect of pH on electrostatic self-assembly of poly(amidoamine) dendrimers of generation 4 and di- and trivalent anionic organic dyes. The solution pH is used as a key to turn on the interaction and to control the association by regulating the macroion charge. Stable and well-defined nanoparticles are formed in solution, being more stable at low pH where the dendrimer protonation is complete. Nanoparticle stability was correlated with ζ-potential measurements. We prove that the assemblies are electrostatically stabilized and elucidate the importance of the surface charge density. pH was also used as a key to nanoparticle dimension and shape. For example, smaller particles form at a lower pH. The nanostructures have been characterized using dynamic light scattering and small-angle neutron scattering. A “phase diagram” has been developed for each dye, showing the assembly size, shape, and instability regions dependent on the pH. Overall, a pH-responsive nanoparticle shape is a key step toward the design of novel smart therapeutic carrier systems.

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    Cited By

    This article is cited by 7 publications.

    1. Jianan Huang, Jiahua Wang, Peng Ding, Wenjuan Zhou, Lei Liu, Xuhong Guo, Martien A. Cohen Stuart, Junyou Wang. Hierarchical Assemblies of Dendrimers Embedded in Networks of Lanthanide-Based Supramolecular Polyelectrolytes. Macromolecules 2019, 52 (4) , 1874-1881. https://doi.org/10.1021/acs.macromol.8b02480
    2. Alexander Zika, Mohit Agarwal, Wiebke Zika, Dirk M. Guldi, Ralf Schweins, Franziska Gröhn. Photoacid-macroion assemblies: how photo-excitation switches the size of nano-objects. Nanoscale 2024, 16 (2) , 923-940. https://doi.org/10.1039/D3NR04570F
    3. Anja Krieger, Alexander Zika, Franziska Gröhn. Functional Nano-Objects by Electrostatic Self-Assembly: Structure, Switching, and Photocatalysis. Frontiers in Chemistry 2022, 9 https://doi.org/10.3389/fchem.2021.779360
    4. Alexander Zika, Anja Krieger, Franziska Gröhn. Nano-Objects by Spontaneous Electrostatic Self-Assembly in Aqueous Solution. 2022, 119-167. https://doi.org/10.1007/978-3-031-00657-9_5
    5. Giacomo Mariani, Anja Krieger, Daniel Moldenhauer, Ralf Schweins, Franziska Gröhn. Light‐Responsive Shape: From Micrometer‐Long Nanocylinders to Compact Particles in Electrostatic Self‐Assembly. Macromolecular Rapid Communications 2018, 39 (17) https://doi.org/10.1002/marc.201700860
    6. Seyed Ali Eghtesadi, Marjan Alsadat Kashfipour, Xinyu Sun, Wei Zhang, Robert Scott Lillard, Stephen Z. D. Cheng, Tianbo Liu. Hierarchical self-assembly of zwitterionic dendrimer–anionic surfactant complexes into multiple stimuli-responsive dynamic nanotubes. Nanoscale 2018, 10 (3) , 1411-1419. https://doi.org/10.1039/C7NR07950H
    7. Giacomo Mariani, Ralf Schweins, Franziska Gröhn. Structure Tuning of Electrostatically Self‐Assembled Nanoparticles through pH: The Role of Charge Ratio. Macromolecular Chemistry and Physics 2017, 218 (24) https://doi.org/10.1002/macp.201700191

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