Synergistic Interactions in Complex Formulations

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Polymer Physics and Theory".

Deadline for manuscript submissions: closed (5 June 2023) | Viewed by 5604

Special Issue Editors


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Guest Editor
Department of Pharmaceutical, Chemical and Environmental Sciences, University of Greenwich, London, UK
Interests: formulation; polymer–surfactant mixtures; polymer–particle interactions; polymer complexation; self-assembly; pulsed-gradient spin-echo NMR; neutron scattering
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Guest Editor
Leicester School of Pharmacy, De Montfort University, The Gateway, Leicester LE1 9BH, UK
Interests: cosmetic science; formulation; complex fluids
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Many formulated systems, e.g., paints, foodstuffs, cosmetics, drug delivery systems, involve heavily engineered formulations that harness synergy between the disparate components to yield some beneficial character during application. Often, such molecular-level interactions are poorly understood.

Invariably, a polymeric component is present in these formulations whose function is to modulate the structure or dynamics of the system, e.g., as a stabilising or rheological agent, but their interaction with other formulation components, e.g., particles or surfactants can lead to unexpected behaviour.

The range of experimental methodologies that can provide direct insights into such complex systems tends to narrow as the number of components increases, without recourse to specifically labelled molecules.

This Special Edition will focus on how synergistic interactions are identified, quantified, and characterised in terms of the many species present in the formulation, highlighting those aspects that are desirable and those are less so.

Prof. Dr. Peter Griffiths
Dr. Omar Mansour
Guest Editors

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Published Papers (3 papers)

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Research

14 pages, 1957 KiB  
Article
Morphological Transitions in Micelles of Amphiphilic Bottlebrushes upon the Adsorption and Compression at the Liquid Interface
by Alina S. Bugaeva, Rustam A. Gumerov and Igor I. Potemkin
Polymers 2022, 14(23), 5076; https://doi.org/10.3390/polym14235076 - 23 Nov 2022
Cited by 1 | Viewed by 1238
Abstract
Densely grafted comb-like macromolecules (bottlebrushes) with alternating solvophobic and solvophilic side chains were studied in a selective solvent and at the liquid interface using mesoscopic computer simulations. The effects of backbone length and copolymer composition were considered. While self-assembly in solution revealed only [...] Read more.
Densely grafted comb-like macromolecules (bottlebrushes) with alternating solvophobic and solvophilic side chains were studied in a selective solvent and at the liquid interface using mesoscopic computer simulations. The effects of backbone length and copolymer composition were considered. While self-assembly in solution revealed only spherical aggregates for all ar-chitectures studied, adsorption onto the liquid interface in particular cases resulted in morpho-logical changes, with worm-like aggregates or a continuous monolayer observed. In turn, the compression of macromolecules at the interface also leads to morphological transitions, includ-ing the formation of a mesh-like percolated structure. The obtained results may be useful for the preparation of solid nanoparticles of anisotropic shape or nanostructured ultra-thin copolymer films. Full article
(This article belongs to the Special Issue Synergistic Interactions in Complex Formulations)
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24 pages, 7091 KiB  
Article
The Effect of Conductive Heat Transfer on the Morphology Formation in Polymer Solutions Undergoing Thermally Induced Phase Separation
by Samira Ranjbarrad and Philip K. Chan
Polymers 2022, 14(20), 4345; https://doi.org/10.3390/polym14204345 - 15 Oct 2022
Cited by 4 | Viewed by 1396
Abstract
Owing to the fact that heat transfer during the thermally induced phase separation process is limited, a quench rate is inevitably entailed, which leads to the existence of temporal and spatial variations in temperature. Hence, it is of great importance to take into [...] Read more.
Owing to the fact that heat transfer during the thermally induced phase separation process is limited, a quench rate is inevitably entailed, which leads to the existence of temporal and spatial variations in temperature. Hence, it is of great importance to take into account the nonisothermality during the phase separation process, especially in high viscosity polymer solutions. In this study, the influence of conductive heat transfer on the morphology formation during the thermally induced phase separation process was investigated theoretically in terms of quench depth, boundary conditions, and enthalpy of demixing to elucidate the interaction between temperature and concentration through incorporating the nonlinear Cahn-Hilliard equation and the Fourier heat transfer equation in two dimensions. The Flory-Huggins free energy theory for the thermodynamics of phase separation, slow mode theory, and Rouse law for polymer diffusion without entanglements were taken into account in the model development. The simulation results indicated a strong interaction between heat transfer and phase separation, which impacted the morphology formation significantly. Results confirmed that quench depth had an indispensable impact on phase separation in terms of higher characteristic frequency by increasing the driving force for heat transfer. Applying quench from various boundaries led to a difference in the quench rate due to the high viscosity of the polymer solution. This led to a gradation in pore size and anisotropic morphology formation. The degree and direction of anisotropy depended on quench depth and rate, quench time, heat conduction rate inside the solution, solution viscosity, temperature evolution, and the enthalpy of demixing. It was also verified that the influence of enthalpy of demixing on phase separation could not be neglected as it increased the solution temperature and led to phase separation being accomplished at a higher temperature than the initial quench temperature. Full article
(This article belongs to the Special Issue Synergistic Interactions in Complex Formulations)
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13 pages, 1631 KiB  
Article
Using Polymer–Surfactant Charge Ratio to Control Synergistic Flocculation of Anionic Particulate Dispersions
by Christopher Hill, Wasiu Abdullahi, Martin Crossman and Peter Charles Griffiths
Polymers 2022, 14(17), 3504; https://doi.org/10.3390/polym14173504 - 26 Aug 2022
Cited by 3 | Viewed by 2353
Abstract
This study investigates the flocculation induced destabilization of particulate dispersions by oppositely charged polymer–surfactant complexes, with a particular focus on controlling interactions by modulating the charge ratio Z, (where Z = [+polymer]/[−surfactant]) via [−surfactant] at fixed [...] Read more.
This study investigates the flocculation induced destabilization of particulate dispersions by oppositely charged polymer–surfactant complexes, with a particular focus on controlling interactions by modulating the charge ratio Z, (where Z = [+polymer]/[−surfactant]) via [−surfactant] at fixed Cpolymer. Cationic hydroxyethyl cellulose (cat-HEC) polymer-sodium dodecylsulfate (SDS) complexes were prepared with either excess polymer (Z > 1) or surfactant (Z < 1) charges. Anionic particulate dispersions (Ludox and polystyrene-butadiene Latex) were then exposed to the complexes, and solvent relaxation NMR was used to characterize the particle surfaces before and after exposure. In both particulate dispersions, flocculation induced destabilization was enhanced after exposure to cat-HEC-SDS complexes with Z > 1, leaving any excess particle surfaces uncoated after gentle centrifugation. However, complexes with Z < 1 showed no adsorption and destabilization in the Ludox dispersions and only slight destabilization in the Latex dispersions due to possible hydrophobic interactions. Substituting SDS for non-ionic surfactant (C12E6) showed no additional destabilization of the dispersions, but post-centrifugation relaxation rates indicated preferential adsorption of C12E6 onto the particle surfaces. Since the dominant forces are electrostatic, this study highlights the possibility of controlling the interactions between oppositely charged polymer–surfactant complexes and particle surfaces by modulating Z through [−surfactant]. Full article
(This article belongs to the Special Issue Synergistic Interactions in Complex Formulations)
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