Single and mixed Pluronics® micelles with solubilized hydrophobic additives: Underscoring the aqueous solution demeanor and micellar transition

This study scrutinizes the self-association of ethylene oxide (EO)-propylene oxide (PO)-based star-shaped block copolymers as normal Tetronic® (T904) and reverse Tetronic® R (T90R4) with varying molecular characteristics and different hydrophilic-hydrophobic ratios in an aqueous solution environment. These thermo-responsive solutions appear clear, transparent or bluish up to 10%w/v, which anticipated the probable transition of unimers to spherical or ellipsoidal micelles which is complemented by scattering experiments. In a single-solution environment, 10%w/v T904 formed star-shaped micelles at ambient temperature and exhibited a micellar growth/transition with temperature ageing. While 10%w/v T90R4 exists as unimers or a Gaussian coil over a wide range of temperature. Very interestingly, close to the cloud point (CP) flower-shaped spherical and ellipsoidal micelles were formed. A similar proposed micellar scheme was also examined for mixed systems T904 : T90R4 in varying ratios (1 : 0, 3 : 1, 1 : 1, 1 : 3 and 0 : 1) giving an account to the solution behavior of the mixtures. An amalgamation of dynamic light scattering (DLS) and small-angle neutron scattering (SANS) techniques achieved the thorough extraction of the structural parameters of the micellar system. The hydrodynamic diameter (Dh) of the micelles with temperature variation was evaluated from dynamic light scattering (DLS) while the structure factor of the micelles was found by employing small-angle neutron scattering (SANS). Furthermore, the single and mixed micellar systems were quantitatively and qualitatively examined for anticancer drug solubilization using UV-vis spectroscopy for their superior use as potential nanocargos.

Micellar assembly leading to structural growth/transition in normal and reverse Tetronics® in single and mixed solution environment.

Poly(ethylene oxide, EO)-poly(propylene oxide, PO)-poly(ethylene oxide, EO)-based triblock copolymers (BCPs) with 80% hydrophilicity stay molecularly dissolved as Gaussian chains at ambient temperature, even at fairly high concentrations (>5 %w/v). This study presents the plausible micellization behaviour of such very-hydrophilic Pluronics® - F38, F68, F88, F98, and F108 - incited upon the addition of glucose at low concentrations and temperatures. The outcomes obtained from phase behaviour and scattering studies are described. At temperatures near to ambient temperature, these BCPs form micelles with a central core made of a PO block, surrounded by a corona of highly hydrated EO chains. The phase transitions in these hydrophilic Pluronics® in the presence of glucose are demonstrated via the dehydration of the copolymer coil, leading to a decrease in the I1/I3 ratio, as determined using fluorescence spectroscopy. The temperature-dependent cloud point (CP) showed a marked decrease with an increase in the PO molecular weight and also in the presence of glucose. The change in solution relative viscosity (ηrel) caused by glucose is due to the enhanced dehydration of the EO block of the BCP amphiphile. Dynamic light scattering (DLS) and small-angle neutron scattering (SANS) investigations suggested that the dimensions of the hydrophobic core increase during the dehydration of the EO-PO blocks upon a temperature increase or after adding varying concentrations of glucose, thereby resulting in a micellar shape transition. It has been observed that added glucose influences the phase behaviour of BCPs in an analogous way to the influence of temperature. Also, plausible interactions between the EO-PO blocks and glucose were suggested based on the evaluated optimized descriptors obtained from a computational simulation approach. In addition, the core-shell blended micelles obtained using these BCPs are successfully utilized for drug (curcumin, Cur) solubilization based on the observed peak intensities from UV-visible spectroscopy. The loading of Cur into glucose-containing and glucose-free hydrophilic Pluronic® micelles shows how the radius of the micellar core (Rc) increases in the presence of glucose, thereby indicating Cur solubility enhancement for the Pluronic® micelles. Various kinetics models were employed, demonstrating a drug release profile that enables this approach to be used as an ideal platform for drug delivery.

Glucose-induced self-assembly and phase separation in hydrophilic triblock copolymers and the governing mechanism.

The nanoscale association domains are the ultimate determinants of the macroscopic properties of complex fluids involving amphiphilic polymers and surfactants, and hence, it is foremost important to understand the role of polymer/surfactant concentration on these domains. We have used coarse-grained molecular dynamics simulations to investigate the effect of polymer/surfactant concentration on the morphology of poly(ethylene oxide)-poly(propylene oxide)-poly(ethylene oxide) (PEO-PPO-PEO, i.e., pluronics or poloxamers) block copolymer, and ionic surfactants sodium dodecyl sulfate (SDS), mixed micelles in aqueous solution. The proclivity of the surfactant to form the mixed micelles is also probed using umbrella sampling simulations. In this study, we observed that the core of the pluronic + SDS formed mixed micelles consists of PPO, the alkyl tail of SDS, and some water molecules, whereas the PEO, water, and sulfate headgroups of SDS form a shell, consistent with experimental observations. The micelles are spherical at high-pluronic/low-SDS compositions, ellipsoidal at high-SDS/low-pluronic compositions, and wormlike-cylindrical at high-pluronic/high-SDS compositions. The transitions in micelle morphology are governed by the solvent accessible surface area of mixed aggregates, electrostatic repulsion between SDS-headgroups, and dehydration of PEO and PPO segments. The free energy barrier for SDS escape is much higher in mixed micelles than in pure SDS micelles, indicating a stronger tendency for SDS to form pluronic-SDS mixed micelles.

Molecular Insights on Morphology, Composition, and Stability of Mixed Micelles Formed by Ionic Surfactant and Nonionic Block Copolymer in Water Using Coarse-Grained Molecular Dynamics Simulations.

Nanoscale Pluronic® micellar templates with varying %EO content for controlled drug release and cytotoxicity

An expedient in to the phase behaviour and scattering profile in PEO-PPO-PEO block copolymer mixed systems in aqueous solution

SDS triggered transformation of highly hydrophobic Pluronics® nanoaggregate into polymer-rich and surfactant-rich mixed micelles

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Single and mixed Pluronics® micelles with solubilized hydrophobic additives: Underscoring the aqueous solution demeanor and micellar transition

An expedient in to the phase behaviour and scattering profile in PEO-PPO-PEO block copolymer mixed systems in aqueous solution

SDS triggered transformation of highly hydrophobic Pluronics® nanoaggregate into polymer-rich and surfactant-rich mixed micelles