Correction to “Integration of Gold Nanoparticles into Bilayer Structures via Adaptive Surface Chemistry”

Lee, Heeyoung; Shin, Song Seok; Abezgauz, Ludmila; Lewis, Sean A.; Chirsan, Aaron M.; Danino, Dganit; Bishop, Kyle J. M.

doi:10.1021/ja407234h

Cited by 5 publications

(7 citation statements)

References 1 publication

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“…In other words, IONPCs do not undergo a full disassembly process because of removal of the acetate/oleate bilayer from the surface; Dynamic rearrangement of the CTA + –oleate bilayer and formation of the tiny gates opening to the hydrophobic cores of IONPCs must have been the driving force for the fusion of nanoemulsions to the IONPCs. This appears to be an accurate scenario because similar fusion interactions of surfactant vesicles to the dynamic ligands on the nanoparticle surfaces are already known . When the fusion process started (Figure G), the hydrophobic phase of silica precursors must have been transferred into the hydrophobic core of the IONPCs, and two hydrophobic phases must have merged inside the clusters (as in the case of coalescence of Janus colloidal capsules).…”

Section: Resultsmentioning

confidence: 87%

“…This appears to be an accurate scenario because similar fusion interactions of surfactant vesicles to the dynamic ligands on the nanoparticle surfaces are already known. 67 When the fusion process started ( Figure 10 G), the hydrophobic phase of silica precursors must have been transferred into the hydrophobic core of the IONPCs, and two hydrophobic phases must have merged inside the clusters (as in the case of coalescence of Janus colloidal capsules 56 ). This could be the explanation why we observed that the emulsions seemed to be invading the IONP clusters in the cryo-TEM images ( Figure 7 A,B).…”

Section: Resultsmentioning

confidence: 99%

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

et al. 2017

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It has been long known that the physical encapsulation of oleic acid-capped iron oxide nanoparticles (OA–IONPs) with the cetyltrimethylammonium (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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Section: Resultsmentioning

confidence: 87%

Section: Resultsmentioning

confidence: 99%

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

et al. 2017

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“…The surface property of these anionic AuNPs was then characterized by titration with a cationic surfactant cetyltrimethylammonium tosylate (CTAT) . Stepwise addition of 1.0 mM CTAT solution to 2.4 nM MUA-AuNPs caused spectroscopically visible aggregation of nanoparticles at the point of overall charge neutrality, monitored by the ratio of absorbance at 650 and 520 nm (Figure d).…”

Section: Resultsmentioning

confidence: 99%

“…This uptake pathway is also applied to other cationic nanoparticles. However, the disruptive nanoparticle–membrane interactions associate, at least partially, with cytotoxicity, which to some extent limits the biomedicine applications of cationic nanoparticles. ,, More recently, researchers found that anionic AuNPs with structured surfaces composed of a binary mixture of hydrophobic and anionic ligands can nondisruptively penetrate cellular membranes, involving a pathway fundamentally different from that of cationic nanoparticles. ,, The ribbon-like distribution of ligands on the surface of Au NPs has been demonstrated to be vital for the nondisruptive penetration of anionic AuNPs through membranes.…”

Section: Introductionmentioning

confidence: 99%

Aromaticity/Bulkiness of Surface Ligands to Promote the Interaction of Anionic Amphiphilic Gold Nanoparticles with Lipid Bilayers

et al. 2016

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The presence of large hydrophobic aromatic residues in cell-penetrating peptides or proteins has been demonstrated to be advantageous for their cell penetration. This phenomenon has also been observed when AuNPs were modified with peptides containing aromatic amino acids. However, it is still not clear how the presence of hydrophobic and aromatic groups on the surface of anionic AuNPs affects their interaction with lipid bilayers. Here, we studied the interaction of a range of anionic amphiphilic AuNPs coated by different combinations of hydrophobic and anionic ligands with four different types of synthetic lipid vesicles. Our results demonstrated the important role of the surface aromatic or bulky groups, relative to the hydrocarbon chains, in the interaction of anionic AuNPs with lipid bilayers. Hydrophobic interaction itself arising from the insertion of aromatic/bulky ligands on the surface of AuNPs into lipid bilayers is sufficiently strong to cause overt disruption of lipid vesicles and cell membranes. Moreover, by comparing the results obtained from AuNPs coated with aromatic ligands and cyclohexyl ligands lacking aromaticity respectively, we demonstrated that the bulkiness of the terminal groups in hydrophobic ligands instead of the aromatic character might be more important to the interaction of AuNPs with lipid bilayers. Finally, we further correlated the observation on model liposomes with that on cell membranes, demonstrating that AuNPs that are more disruptive to the more negatively charged liposomes are also substantially more disruptive to cell membranes. In addition, our results revealed that certain cellular membrane domains that are more susceptible to disruption caused by hydrophobic interactions with nanoparticle surfaces might determine the threshold of AuNP-mediated cytotoxicity.

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“…Exploring the role that particle surface coatings have on these interactions is of central importance. For particles with uniform surface chemistry, surface properties such as charge, − hydrophobicity, − and adsorbed protein corona − have been shown to play pivotal roles in determining their interaction with biomembranes. Much less is known about the effects of heterogeneous surface chemistry.…”

mentioning

confidence: 99%

Rupture of Lipid Membranes Induced by Amphiphilic Janus Nanoparticles

Lee

Zhang

et al. 2018

ACS Nano

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The surface coatings of nanoparticles determine their interaction with biomembranes, but studies have been limited almost exclusively to nanoparticles with a uniform surface chemistry. Although nanoparticles are increasingly made with complex surface chemistries to achieve multifunctionalities, our understanding of how a heterogeneous surface coating affects particle-biomembrane interaction has been lagging far behind. Here we report an investigation of this question in an experimental system consisting of amphiphilic "two-faced" Janus nanoparticles and supported lipid membranes. We show that amphiphilic Janus nanoparticles at picomolar concentrations induce defects in zwitterionic lipid bilayers. In addition to revealing the various effects of hydrophobicity and charge in particle-bilayer interactions, we demonstrate that the Janus geometry-the spatial segregation of hydrophobicity and charges on particle surface-causes nanoparticles to bind more strongly to bilayers and induce defects more effectively than particles with uniformly mixed surface functionalities. We combine experiments with computational simulation to further elucidate how amphiphilic Janus nanoparticles extract lipids to rupture intact lipid bilayers. This study provides direct evidence that the spatial arrangement of surface functionalities on a nanoparticle, rather than just its overall surface chemistry, plays a crucial role in determining how it interacts with biological membranes.

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Correction to “Integration of Gold Nanoparticles into Bilayer Structures via Adaptive Surface Chemistry”

Cited by 5 publications

References 1 publication

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

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

Aromaticity/Bulkiness of Surface Ligands to Promote the Interaction of Anionic Amphiphilic Gold Nanoparticles with Lipid Bilayers

Rupture of Lipid Membranes Induced by Amphiphilic Janus Nanoparticles

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