Unraveling the Phase Behavior, Mechanical Stability, and Protein Reconstitution Properties of Polymer–Lipid Hybrid Vesicles

Müller, Wagner Augusto; Beales, Paul A.; Muniz, André R.; Jeuken, Lars J. C.

doi:10.1021/acs.biomac.3c00498

Cited by 3 publications

(2 citation statements)

References 80 publications

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“…Except for the systems integrating P(OEGMA- co -LMA)-1, there are also spherical or irregular-shaped vesicles of 20–100 nm with a thinner membrane and a better imaging contrast of 6 nm—still a little larger than that of neat liposomes (≤5 nm) evidencing a hybrid bilayer with a different conformation of the copolymer. 56 − 58 However, Dao et al (2017) indicated that pure DPPC vesicles were accompanied by a membrane of 6 nm. 51 Reasonably, we could not exclude the scenario that the membrane of these structures corresponds to neat lipid bilayers.…”

Section: Resultsmentioning

confidence: 99%

“…This finding suggests that the copolymers were effectively incorporated into the lipid bilayer, and mixed structures were created. 30,51,53,55 Muller et al 56 confirmed the increase of membrane thickness due to different configuration of the copolymer in a lipid-to-polymer ratio-dependent manner. In this study, the membrane thickness does not seem to be influenced by the % weight of the copolymer in the systems.…”

Section: Exploring the Morphology Of Lipid/copolymermentioning

confidence: 94%

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Deciphering the Lipid-Random Copolymer Interactions and Encoding Their Properties to Design a Hybrid System

Triantafyllopoulou,

Forys,

Perinelli

et al. 2024

Langmuir

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Lipid/copolymer colloidal systems are deemed hybrid materials with unique properties and functionalities. Their hybrid nature leads to complex interfacial phenomena, which have not been fully encoded yet, navigating their properties. Moving toward in-depth knowledge of such systems, a comprehensive investigation of them is imperative. In the present study, hybrid lipid/copolymer structures were fabricated and examined by a gamut of techniques, including dynamic light scattering, fluorescence spectroscopy, cryogenic transmission electron microscopy, microcalorimetry, and high-resolution ultrasound spectroscopy. The biomaterials that were mixed for this purpose at different ratios were 1,2-dioctadecanoyl-sn-glycero-3-phosphocholine and four different linear, statistical (random) amphiphilic copolymers, consisting of oligo(ethylene glycol) methyl ether methacrylate as the hydrophilic comonomer and lauryl methacrylate as the hydrophobic one. The colloidal dispersions were studied for lipid/copolymer interactions regarding their physicochemical, morphological, and biophysical behavior. Their membrane properties and interactions with serum proteins were also studied. The aforementioned techniques confirmed the hybrid nature of the systems and the location of the copolymer in the structure. More importantly, the random architecture of the copolymers, the hydrophobic-to-hydrophilic balance of the nanoplatforms, and the lipid-to-polymer ratio are highlighted as the main design-influencing factors. Elucidating the lipid/copolymer interactions would contribute to the translation of hybrid nanoparticle performance and, thus, their rational design for multiple applications, including drug delivery.

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Section: Resultsmentioning

confidence: 99%

Section: Exploring the Morphology Of Lipid/copolymermentioning

confidence: 94%

Deciphering the Lipid-Random Copolymer Interactions and Encoding Their Properties to Design a Hybrid System

Triantafyllopoulou,

Forys,

Perinelli

et al. 2024

Langmuir

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Hybrid lipid-block copolymer membranes enable stable reconstitution of a wide range of nanopores and robust sampling of serum

Vreeker,

Grünewald,

van der Heide

et al. 2024

Preprint

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Biological nanopores are powerful tools for detecting biomolecules at the single-molecule level, making them appealing as sensors for biological samples. However, the lipid membranes in which nanopores reside can be unstable in the presence of biological fluids. Here, membranes formed with the amphiphilic polymers PMOXA-PDMS-PMOXA and PBD-PEO are tested as potential alternatives for nanopore sensing. We demonstrate that polymer membranes can possess increased stability towards applied potentials and high concentrations of human serum, but that the stable insertion of a wide range of biological nanopores is most often compromised. Alternatively, hybrid polymer-lipid membranes comprising a 1:1 w/w mixture of PBD11PEO8 and DPhPC showed high electrical and biochemical stability while creating a suitable environment for all tested nanopores. Analytes such as proteins, DNA and sugars were efficiently sampled, indicating that in hybrid membranes nanopores showed native-like properties. Molecular dynamics simulations revealed that lipids form ~12 nm domains interspersed by a polymer matrix. Nanopores partitioned into these lipid nanodomains and sequestered lipids possibly offering the same binding strength as in a native bilayer. This work shows that single-molecule analysis with nanopores in [PBD11PEO8 + DPhPC] membranes is feasible and present stable recordings in the presence of human serum. These results pave the way towards novel nanopore-based biosensors.

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Unveiling the Performance of Co-Assembled Hybrid Nanocarriers: Moving towards the Formation of a Multifunctional Lipid/Random Copolymer Nanoplatform

Triantafyllopoulou,

Perinelli,

Forys

et al. 2024

Pharmaceutics

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Despite the appealing properties of random copolymers, the use of these biomaterials in association with phospholipids is still limited, as several aspects of their performance have not been investigated. The aim of this work is the formulation of lipid/random copolymer platforms and the comprehensive study of their features by multiple advanced characterization techniques. Both biomaterials are amphiphilic, including two phospholipids (1,2-dioctadecanoyl-sn-glycero-3-phosphocholine (DSPC), 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC)) and a statistical copolymer of oligo (ethylene glycol) methyl ether methacrylate (OEGMA) and 2-(diisopropylamino) ethyl methacrylate (DIPAEMA). We examined the design parameters, including the lipid composition, the % comonomer ratio, and the lipid-to-polymer ratio that could be critical for their behavior. The structures were also probed in different conditions. To the best of the authors’ knowledge, this is the first time that P(OEGMA-co-DIPAEMA)/lipid hybrid colloidal dispersions have been investigated from a membrane mechanics, biophysical, and morphological perspective. Among other parameters, the copolymer architecture and the hydrophilic to hydrophobic balance are deemed fundamental parameters for the biomaterial co-assembly, having an impact on the membrane’s fluidity, morphology, and thermodynamics. Exploiting their unique characteristics, the most promising candidates were utilized for methotrexate (MTX) loading to explore their encapsulation capability and potential antitumor efficacy in vitro in various cell lines.

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Unraveling the Phase Behavior, Mechanical Stability, and Protein Reconstitution Properties of Polymer–Lipid Hybrid Vesicles

Cited by 3 publications

References 80 publications

Deciphering the Lipid-Random Copolymer Interactions and Encoding Their Properties to Design a Hybrid System

Deciphering the Lipid-Random Copolymer Interactions and Encoding Their Properties to Design a Hybrid System

Hybrid lipid-block copolymer membranes enable stable reconstitution of a wide range of nanopores and robust sampling of serum

Unveiling the Performance of Co-Assembled Hybrid Nanocarriers: Moving towards the Formation of a Multifunctional Lipid/Random Copolymer Nanoplatform

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