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Light-weight paper products that contain less fibres, but with a maintained bulk and improved strength properties, are highly desirable due to the low cost of raw materials and improved logistics of packaged goods. In this respect, the adsorption capacity of dry strength additives onto fibres, which is affected by the surface charge of said fibres, is very important for the development of these mechanically robust paper products. The influence of the surface charge on the adsorption of strength additives was investigated for, dissolving grade fibres, kraft fibres and kraft fibres modified with carboxymethyl cellulose (CMC) with different surface charge densities, but the same fibre dimensions. The strength additives investigated were cationic starch (CS), anionic polyacrylamide (APAM) and polyelectrolyte complexes (PECs), containing CS and APAM. A linear relationship was found between the surface charge of the fibres and the saturated adsorbed amount of CS. However, when either APAM or PECs adsorbed as secondary layers onto the CS, no correlation between cellulose charge and the saturation adsorption could be observed. The adsorption of APAM was dramatically affected by the pre-adsorbed amount of CS, whereas PECs were less influenced. Moreover, the additives improved the tensile strength (60%) and strain at break (> 100%) of handsheets formed with the kraft fibres and adsorbed APAM. It was also found that CS/APAM increased the sheet density while CS/PECs lowered it. In conclusion, the gained fundamental understanding of these adsorption of additives is of significant importance to facilitate the industrial development of sustainable low-cost high-end packaging products. Graphical abstract

This study aimed to develop nanovectors co-encapsulating doxorubicin (Doxo) and zoledronic acid (Zol) for a combined therapy against Doxo-resistant tumors. Chitosan (CHI)-based polyelectrolyte complexes (PECs) prepared by ionotropic gelation technique were proposed. The influence of some experimental parameters was evaluated in order to optimize the PECs in terms of size and polydispersity index (PI). PEC stability was studied by monitoring size and zeta potential over time. In vitro studies were carried out on wild-type and Doxo-resistant cell lines, to assess both the synergism between Doxo and Zol, as well as the restoring of Doxo sensitivity. Polymer concentration, incubation time, and use of a surfactant were found to be crucial to achieving small size and monodisperse PECs. Doxo and Zol, only when encapsulated in PECs, showed a synergistic antiproliferative effect in all the tested cell lines. Importantly, the incubation of Doxo-resistant cell lines with Doxo/Zol co-encapsulating PECs resulted in the restoration of Doxo sensitivity.

There is notable discrepancy between experiments and coarse-grained model studies regarding the thermodynamic driving force in polyelectrolyte complex coacervation: experiments find the free energy change to be dominated by entropy, while simulations using coarse-grained models with implicit solvent usually report a large, even dominant energetic contribution in systems with weak to intermediate electrostatic strength. Here, using coarse-grained, implicit-solvent molecular dynamics simulation combined with thermodynamic analysis, we study the potential of mean force (PMF) in the two key stages on the coacervation pathway for symmetric polyelectrolyte mixtures: polycation–polyanion complexation and polyion pair–pair condensation.We show that the temperature dependence in the dielectric constant of water gives rise to a substantial entropic contribution in the electrostatic interaction. By accounting for this electrostatic entropy, which is due to solvent reorganization, we find that under common conditions (monovalent ions, room temperature) for aqueous systems, both stages are strongly entropy-driven with negligible or even unfavorable energetic contributions, consistent with experimental results. Furthermore, for weak to intermediate electrostatic strengths, this electrostatic entropy, rather than the counterion-release entropy, is the primary entropy contribution. From the calculated PMF, we find that the supernatant phase consists predominantly of polyion pairs with vanishingly small concentration of bare polyelectrolytes, and we provide an estimate of the spinodal of the supernatant phase. Finally, we showthat prior to contact, two neutral polyion pairsweakly attract each other by mutually induced polarization, providing the initial driving force for the fusion of the pairs.

Chitosan is a cationic polysaccharide that is usually obtained by alkaline deacetylation of chitin poly(N-acetylglucosamine). It is biocompatible, biodegradable, mucoadhesive, and non-toxic. These excellent biological properties make chitosan a good candidate for a platform in developing drug delivery systems having improved biodistribution, increased specificity and sensitivity, and reduced pharmacological toxicity. In particular, chitosan nanoparticles are found to be appropriate for non-invasive routes of drug administration: oral, nasal, pulmonary and ocular routes. These applications are facilitated by the absorption-enhancing effect of chitosan. Many procedures for obtaining chitosan nanoparticles have been proposed. Particularly, the introduction of hydrophobic moieties into chitosan molecules by grafting to generate a hydrophobic-hydrophilic balance promoting self-assembly is a current and appealing approach. The grafting agent can be a hydrophobic moiety forming micelles that can entrap lipophilic drugs or it can be the drug itself. Another suitable way to generate self-assembled chitosan nanoparticles is through the formation of polyelectrolyte complexes with polyanions. This paper reviews the main approaches for preparing chitosan nanoparticles by self-assembly through both procedures, and illustrates the state of the art of their application in drug delivery.

Biopolymers have several advantages for the development of drug delivery systems, since they are biocompatible, biodegradable and easy to obtain from renewable resources. However, their most notable advantage may be their ability to adhere to biological tissues. Many of these biopolymers have ionized forms, known as polyelectrolytes. When combined, polyelectrolytes with opposite charges spontaneously form polyelectrolyte complexes or multilayers, which have great functional versatility. Although only one natural polycation—chitosan has been widely explored until now, it has been combined with many natural polyanions such as pectin, alginate and xanthan gum, among others. These polyelectrolyte complexes have been used to develop multiple mucoadhesive dosage forms such as hydrogels, tablets, microparticles, and films, which have demonstrated extraordinary potential to administer drugs by the ocular, nasal, buccal, oral, and vaginal routes, improving both local and systemic treatments. The advantages observed for these formulations include the increased bioavailability or residence time of the formulation in the administration zone, and the avoidance of invasive administration routes, leading to greater therapeutic compliance.

A novel chitosan/alginate composite membrane is proposed for the application of greywater treatment. In particular, the effect of stirring speed of mixing chitosan and alginate solution was investigated in this study. The study revealed that 150CSAL and 210CSAL membranes swell significantly compared to CS membrane due to the porous structure of composite membrane. The FTIR spectra revealed that the mixing speed has no influence in terms of molecular interaction between CS and AL due to fixed CS and AL concentrations used in this study. On the other hand, the complexation of AL with CS made outstanding improvement to the dense structure of CS where 180CSAL membrane has UP water flux as high as 90 L/m2h at 2 bar. All membranes have the capability to remove the pollutants present in GW and the COD removal was further improved up to 7% using CSAL membranes. In addition, increasing mixing speed improved the pathogen removal efficiency compared to CS membrane. The treated GW met the non-potable GW reuse standard for turbidity<5 NTU and TSS<20 mg/L. To summarize, the proposed fabrication technique on CSAL membrane showed improved characteristics to CS membrane and has significant performance on GW treatment.

Biomaterials based on polyelectrolyte complexation are an innovative concept of coatings and packaging production to be applied in a wide range of food products. The aim of this study was to obtain and characterize a sodium alginate–chitosan complex material with variable degree of polyion interactions by complexation of oppositely charged polysaccharides. In order to characterize polyelectrolyte complexes, theromogravimetric analysis (TGA), dynamic mechanical thermal analysis (DMTA), nuclear magnetic resonance (NMR), Fourier transform infrared spectroscopy (FT-IR), matrix-assisted laser desorption/ionization technique with time of flight analyzer (MALDI-TOF), and scanning electron microscopy (SEM) were performed. TGA analysis showed that thermal decomposition temperature depends on the polymer ratio (R) and thermal resistance of samples was improved by increasing chitosan dosage. Accordingly to DMTA results, polyelectrolyte complexation led to obtain more flexible and resistant to mechanical deformation materials. Comparative analysis of the FTIR spectra of single polyelectrolytes, chitosan and alginate, and their mixtures indicated the formation of the polyelectrolyte complex without addition of reinforcing substances. MALDI-TOF analysis confirms the creation of polyelectrolyte aggregates (~197 Da) in samples with R ≥ 0.8; and their chemical stability and safety were proven by NMR analysis. The higher R the greater the number of polyanion–polycation aggregates seen in SEM as film morphology roughness.

To develop an effective pH-sensitive drug carrier, alginate (Alg), carboxymethyl chitosan (CMCs), and aminated chitosan (AmCs) derivatives were employed in this study. A simple ionic gelation technique was employed to formulate Alg-CMCs@AmCs dual polyelectrolyte complexes (PECs) microcapsules as a pH-sensitive carrier for efficient encapsulation and release of diclofenac sodium (DS) drug. The developed microcapsules were characterized by Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analyzer (TGA), and scanning electron microscope (SEM). The results clarified that formation of dual PECs significantly protected Alg microcapsules from rapid disintegration at colon conditions (pH 7.4), and greatly reduced their porosity. In addition, the dual PECs microcapsules can effectively encapsulate 95.4% of DS-drug compared to 86.3 and 68.6% for Alg and Alg-CMCs microcapsules, respectively. Higher DS-release values were achieved in simulated colonic fluid [SCF; pH 7.4] compared to those obtained in simulated gastric fluid [SGF; pH 1.2]. Moreover, the drug burst release was prevented and a sustained DS-release was achieved as the AmCs concentration increased. The results confirmed also that the developed microcapsules were biodegradable in the presence of the lysozyme enzyme. These findings emphasize that the formulated pH-sensitive microcapsules could be applied for the delivery of diclofenac sodium.

It is well known that polyelectrolyte complexes and coacervates can form on mixing oppositely charged polyelectrolytes in aqueous solutions, due to mainly electrostatic attraction between the oppositely charged polymers. Here, we report the first (to the best of our knowledge) complexation and coacervation of two positively charged polyelectrolytes, which provides a new paradigm for engineering strong, self-healing interactions between polyelectrolytes underwater and a new marine mussel-inspired underwater adhesion mechanism. Unlike the conventional complex coacervate, the like-charged coacervate is aggregated by strong short-range cation–π interactions by overcoming repulsive electrostatic interactions. The resultant phase of the like-charged coacervate comprises a thin and fragile polyelectrolyte framework and round and regular pores, implying a strong electrostatic correlation among the polyelectrolyte frameworks. The like-charged coacervate possesses a very low interfacial tension, which enables this highly positively charged coacervate to be applied to capture, carry, or encapsulate anionic biomolecules and particles with a broad range of applications.

Polyelectrolyte multilayers (PEMs) represent a group of polyelectrolyte complex (PEC)–based materials widely investigated in the biomedical and pharmaceutical sciences. Despite the unflagging popularity of the aforementioned systems in tissue engineering, only a few updated scientific reports concerning PEM potential in drug administration can be found. In fact, PEM coatings are currently recognized as important tools for functionalizing implantable scaffolds; however, only a small amount of attention has been given to PEMs as drug delivery materials. Scientific reports on PEMs reveal two dominant reasons for the limited usability of multilayers in pharmaceutical technology: complex and expensive preparation techniques as well as high sensitivity of interacting polyelectrolytes to the varieties of internal and external factors. The aim of this work was to analyze the latest approaches, concerning the potential of PEMs in pharmacy, chemical technology, and (primarily) tissue engineering, with special attention given to possible polymer combinations, technological parameters, and physicochemical characteristics, such as hydrophilicity, adhesive and swelling properties, and internal/external structures of the systems formed. Careful recognition of the above factors is crucial in the development of PEM-based drug delivery materials.