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Droplet Core Intermolecular Interactions and Block Copolymer Composition Heavily Influence Oil-In-Water Nanoemulsion Stability.

ABSTRACT: Colloidal oil-in-water nanoemulsions are gaining increasing interest as a nanoparticle delivery system because of their large oil droplet core that can carry a large payload. In order to formulate these particles with long-term stability, an appropriate oil media and block copolymer pair must be selected. The interaction between the nanoemulsion core and the polymer shell is critical to forming stable nanoparticles. Herein, we probed how interactions between various polymers with hydrocarbon and perfluorocarbon oil media influenced nanoemulsion formation, stability, and size. Through a series of nanoemulsions with unique polymer/oil media combinations, we examined the effects of oil core hydrophobicity, fluorophilicity, surface charge, and volume as well as the effects of polymer tail composition. Surprisingly, we found that nanoemulsions formulated with pure perfluorocarbon oil cores versus perfluoro poly(ether) oil cores exhibited very different characteristics. We also found that both hydrocarbon and fluorocarbon polymer tails interacted favorably with perfluoro poly(ethers) as well as hydrocarbon oil cores forming stable nanoemulsions. We believe these results are focused on the unique properties of perfluorocarbons especially their rigidity, low polarizability, and near-zero surface charge. Interestingly, we saw that perfluoro poly(ethers) deviated from these expected properties resulting in an increased versatility when formulating nanoemulsions with perfluoro poly(ether) oil cores compared to pure perfluorocarbon oil cores. Nanoemulsion size, stability, growth rate, and life time were explored to probe these factors. Experimental and computational data are presented as a rationale.

SUBMITTER: Barres AR

PROVIDER: S-EPMC7454039 | biostudies-literature | 2019 Oct

REPOSITORIES: biostudies-literature

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Droplet Core Intermolecular Interactions and Block Copolymer Composition Heavily Influence Oil-In-Water Nanoemulsion Stability.

Barres Alexa R AR Molugu Sudheer K SK Stewart Phoebe L PL Mecozzi Sandro S

Langmuir : the ACS journal of surfaces and colloids 20190918 39

Colloidal oil-in-water nanoemulsions are gaining increasing interest as a nanoparticle delivery system because of their large oil droplet core that can carry a large payload. In order to formulate these particles with long-term stability, an appropriate oil media and block copolymer pair must be selected. The interaction between the nanoemulsion core and the polymer shell is critical to forming stable nanoparticles. Herein, we probed how interactions between various polymers with hydrocarbon and ...[more]

PMID: 31532686

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Project description:Interest in nanoemulsion technology has increased steadily in recent years for its widespread applications in the delivery of pharmaceuticals, nutraceuticals, and cosmeceuticals. Rational selection of the composition and the preparation method is crucial for developing a stable nanoemulsion system with desired physicochemical characteristics. In the present study, we investigate the influence of intricate factors including composition and preparation conditions that affect characteristic parameters and the stability of the nanoemulsion formation prepared by the spontaneous emulsification method. Octanoic acid, capryol 90, and ethyl oleate were selected to represent oil phases of different carbon-chain lengths. We explored the impact of the addition mode of the oil-Smix phase and aqueous phase, vortexing time, Km (surfactant/cosurfactant) ratio, and the replacement of water by buffers of different pH as an aqueous system. The phase behavior study showed that the Smix phase had a significant impact on the nanoemulsifying ability of the nanoemulsions composed of oil phases of varying carbon-chain lengths. The mode of mixing of the oil-Smix phase to the aqueous phase markedly influenced the mean droplet size and size distribution of the nanoemulsions composed of oil phases as capryol 90. Vortexing time also impacted the mean droplet size and the stability of the generated nanoemulsion system depending on the varying carbon-chain length of the oil phase. The replacement of the water phase by aqueous buffers of pH 1.2, 5.5, 6.8, and 7.4 has altered the mean droplet size and size distribution of the nanoemulsion system. Further, the Km ratio also had a significant influence on the formation of the nanoemulsion system. The findings of this investigation are useful in understanding how the formulation composition and process parameters of the spontaneous emulsification technique are responsible for affecting the physicochemical characteristics and stability of the nanoemulsion system composed of oil of varying carbon-chain (C8-C18) length.

Project description:A poly(N,N'-dimethylacrylamide) (PDMAC) precursor is chain-extended via reversible addition-fragmentation chain transfer (RAFT) aqueous dispersion polymerization of diacetone acrylamide (PDAAM) to produce PDMAC77-PDAAM40 spherical nanoparticles. Post-polymerization core-crosslinking of such nanoparticles was performed at 20 °C, and the resulting covalently stabilized nanoparticles survive exposure to methanol. The linear and core-crosslinked nanoparticles were subjected to high-shear homogenization in turn in the presence of n-dodecane to form macroemulsions. Subsequent processing of these macroemulsions via high-pressure microfluidization produced nanoemulsions. When using the core crosslinked nanoparticles, the droplet diameter was strongly dependent on the copolymer concentration. This indicates that such nanoparticles remain intact under the processing conditions, leading to formation of genuine Pickering nanoemulsions with a z-average diameter of 244 ± 60 nm. In contrast, the linear nanoparticles undergo disassembly to afford molecularly dissolved diblock copolymer chains, which stabilize oil droplets of 170 ± 59 nm diameter. The long-term stability of these two types of n-dodecane-in-water nanoemulsions with respect to Ostwald ripening was examined using analytical centrifugation. When prepared at the same copolymer concentration, Pickering nanoemulsions stabilized by core-crosslinked nanoparticles proved to be significantly more stable than the nanoemulsion stabilized by the amphiphilic PDMAC77-PDAAM40 chains. Moreover, higher copolymer concentrations led to a significantly faster rate of droplet growth. This is attributed to excess copolymer facilitating the diffusion of n-dodecane through the aqueous phase. Finally, analytical centrifugation is used to assess the long-term stability of the analogous squalane-in-water nanoemulsions. These systems are much more stable than the corresponding n-dodecane-in-water nanoemulsions, regardless of whether the copolymer is adsorbed as sterically stabilized nanoparticles or surface-active chains.

Dataset Information

Droplet Core Intermolecular Interactions and Block Copolymer Composition Heavily Influence Oil-In-Water Nanoemulsion Stability.

Publications

Droplet Core Intermolecular Interactions and Block Copolymer Composition Heavily Influence Oil-In-Water Nanoemulsion Stability.

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