Multicompartment dendrimicelles with binary, ternary and quaternary core composition

Kaup, Rebecca; Hove, Jan Bart ten; Bunschoten, Anton; Leeuwen, F.W.B. van; Velders, Aldrik H.

doi:10.1039/d1nr04556c

Cited by 7 publications

(15 citation statements)

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“…At the same time, these data also prove that different dendrimer generations can be encapsulated within one micelle core, in line with our previous work in which differently functionalized dendrimers of the same generation were incorporated inside a single micelle core. 32 …”

Section: Resultsmentioning

confidence: 99%

“…Functionalization was done as described previously. 32 Briefly, 2 mg of PAMAM dendrimers of generation 4, 5, or 6 in methanol were added to a vial. Amounts of 4–6 mol equiv of fluorescein isothiocyanate (FITC) or rhodamine B isothiocyanate (RITC) with respect to the dendrimers were dissolved in 1 mL of methanol and added dropwise to the dendrimer solution, with mixing.…”

Section: Methodsmentioning

confidence: 99%

“…FRET is an ideal methodology to prove exchange between micellar core components, as energy transfer is only possible when the donor and acceptor are in close proximity: i.e., within the same micelle core. 32 In four different kinds of experiments we reveal the exchange properties of dendrimicelles based on dendrimer generations 4, 5, and 6, with, respectively, 64, 128, and 256 positive charges based on the theoretical maximum number of amine end groups. First, the formation of dendrimicelles is proven with DLS and nuclear magnetic resonance (NMR) spectroscopy.…”

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confidence: 99%

“… 28 − 31 Recently, we proved the formation of multicompartment dendrimicelles with up to four different generation 6 dendrimers within one micellar core, by the combined use of cryoTEM and FRET. 32 …”

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confidence: 99%

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Controlling Trapping, Release, and Exchange Dynamics of Micellar Core Components

Kaup

Velders

2022

ACS Nano

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Whereas the formation and overall stability of hierarchically organized self-assembled supramolecular structures have been extensively investigated, the mechanistic aspects of subcomponent dynamics are often poorly understood or controlled. Here we show that the dynamics of polyamidoamine (PAMAM) dendrimer based micelles can be manipulated by changes in dendrimer generation, pH, and stoichiometry, as proven by NMR and FRET. For this, dendrimers were functionalized with either fluorescein (donor) or rhodamine (acceptor) and encapsulated into separate micelles. Upon mixing, exchange of dendrimers is revealed by an increase in FRET. While dendrimicelles based on dendrimer generations 4 and 5 show a clear increase in FRET in time, revealing the dynamic exchange of dendrimers between micellar cores, generation 6 based micelles appear to be kinetically trapped systems. Interestingly, generation 6 based dendrimicelles prepared at a pH of 7.8 rather than 7.0 do show exchange dynamics, which can be attributed to about 25% less charge of the dendrimer, corresponding to the charge of a virtual generation 5.5 dendrimer at neutral pH. Changing the pH of dendrimicelle solutions prepared at a pH of 7.8 to 7.0 shows the activated release of dendrimers. High-resolution NMR spectra of the micellar core are obtained from a 1.2 GHz spectrometer with sub-micromolar sensitivity, with DOSY discriminating released dendrimers from dendrimers still present in the micellar core. This study shows that dendrimer generation, charge density, and stoichiometry are important mechanistic factors for controlling the dynamics of complex coacervate core micelles. This knowledge can be used to tune micelles between kinetically trapped and dynamic systems, with tuning of exchange and/or release speeds, to be tailored for applications in, e.g., material science, sensors, or drug delivery.

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Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

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confidence: 99%

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confidence: 99%

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Controlling Trapping, Release, and Exchange Dynamics of Micellar Core Components

Kaup

Velders

2022

ACS Nano

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“…Interestingly, the mimicking of the role, structure, and properties of molecular systems present in nature (e.g., chlorophyll) can be seen, to some extent, reflected [169]. Very recently, a novel strategy has been used to prepare complex coacervated core micelles by compatibilizing four types of dendrimers containing different cores [170]. Studies show that these mesoscale structures have a hydrodynamic radius and a core size on the nanometer scale.…”

Section: Dendrimer-based Molecular Systems For Fret Phenomenonmentioning

confidence: 99%

Chromophoric Dendrimer-Based Materials: An Overview of Holistic-Integrated Molecular Systems for Fluorescence Resonance Energy Transfer (FRET) Phenomenon

et al. 2021

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Dendrimers (from the Greek dendros → tree; meros → part) are macromolecules with well-defined three-dimensional and tree-like structures. Remarkably, this hyperbranched architecture is one of the most ubiquitous, prolific, and recognizable natural patterns observed in nature. The rational design and the synthesis of highly functionalized architectures have been motivated by the need to mimic synthetic and natural-light-induced energy processes. Dendrimers offer an attractive material scaffold to generate innovative, technological, and functional materials because they provide a high amount of peripherally functional groups and void nanoreservoirs. Therefore, dendrimers emerge as excellent candidates since they can play a highly relevant role as unimolecular reactors at the nanoscale, acting as versatile and sophisticated entities. In particular, they can play a key role in the properties of light-energy harvesting and non-radiative energy transfer, allowing them to function as a whole unit. Remarkably, it is possible to promote the occurrence of the FRET phenomenon to concentrate the absorbed energy in photoactive centers. Finally, we think an in-depth understanding of this mechanism allows for diverse and prolific technological applications, such as imaging, biomedical therapy, and the conversion and storage of light energy, among others.

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Polymeric Dendrimers as Nanocarrier Vectors for Neurotheranostics

Zha

Liu

et al. 2022

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immune responses, activating cellular machinery causing cell stress, cytotoxicity, lack of selectivity, increasing the likelihood of replication competence, and the constrained structure of insert-size, which can limit their biological and medical applications. [2][3][4] By contrast, various forms of nonviral vectors are widely developed and applied in biomedical research because of their low immunogenicity, high biocompatibility, simplicity in structural pattern, ease of size adjustment, practicality in designing various active sites, and low cost of production. [5,6] The most widely studied nonviral vectors are liposomes, inorganic nanoparticles, polymers, and dendrimers. [7] Liposomes are small spherical vesicles from cholesterol and phospholipids characterized with the surface that can be modified using glycolipids or sialic acid. Yet, the unmodified forms of liposomes are structurally unstable and could easily be eliminated by means of body circulation. [8] In this situation, stable inorganic nanoparticles, such as calcium phosphate (Ca 3 (PO 4 ) 2 ), gold (Au), iron oxide (Fe 3 O 4 ), and lanthanide-based nanoparticles are widely used, mainly due to their good hydrophilicity and excellent biocompatibility. [9][10][11] Depending on their chemical core composition, these inorganic nanoparticles display different properties and efficiencies. Lately, inorganic nanoparticles have been developed as effective drug delivery systems and used in many diagnostic techniques. [12] In addition, polymers are widely used as nonviral vectors as well. [13][14][15] Polymers are biodegradable nanomaterials with stable and easily modifiable 3D structures. Their uncomplicated synthesis process allows for large-scale production and safe clinical use compared to inorganic nanoparticles. [16] Notably, dendrimers are hyperbranched polymers with a well-defined chemical structure: a core at the center occupied by array of convergent reactive chain-ends and surface that can easily be modified. [17] The chemistry of dendrimers was first described by Buhleier et al. in 1978. [18] In 1985, Tomalia et al. reported a newer kind of dendrimers based on the mixture of amines and amides, termed polyamidoamine (PAMAM) dendrimers. [19] Dendrimers are intermeshed synthetic organic macromolecules with 3D architecture composition and abundant terminal functional groups. They are well-defined monodispersity-sized materials with extraordinary membrane interaction properties Dendrimers are polymers with well-defined 3D branched structures that are vastly utilized in various neurotheranostics and biomedical applications, particularly as nanocarrier vectors. Imaging agents can be loaded into dendrimers to improve the accuracy of diagnostic imaging processes. Likewise, combining pharmaceutical agents and anticancer drugs with dendrimers can enhance their solubility, biocompatibility, and efficiency. Practically, by modifying ligands on the surface of dendrimers, effective therapeutic and diagnostic platforms can be constructed and implemented for target...

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Multicompartment dendrimicelles with binary, ternary and quaternary core composition

Abstract: Hierarchically built-up multicompartment nanoaggregate systems are of interest for, e.g., novel materials and medicine. Here we present a versatile strategy to generate and unambiguously characterize complex coacervate-core micelles by exploiting...

Cited by 7 publications

References 60 publications

Controlling Trapping, Release, and Exchange Dynamics of Micellar Core Components

Controlling Trapping, Release, and Exchange Dynamics of Micellar Core Components

Chromophoric Dendrimer-Based Materials: An Overview of Holistic-Integrated Molecular Systems for Fluorescence Resonance Energy Transfer (FRET) Phenomenon

Polymeric Dendrimers as Nanocarrier Vectors for Neurotheranostics

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