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Macromolecules and Hydrogel Formulations: Synthesis, Characterization, Pharmacological Effects and Possible Environmental Applications

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A special issue of International Journal of Molecular Sciences (ISSN 1422-0067). This special issue belongs to the section "Macromolecules".

Deadline for manuscript submissions: closed (15 October 2023) | Viewed by 14379

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Prof. Dr. Silvana Alfei

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Department of Pharmacy, University of Genoa, Viale Cembrano, 16148 Genoa, Italy
Interests: nanomaterials; dendrimers; macromolecules; hydrogels for biomedical and environmental applications; resins; polymeric drug delivery systems; organic synthesis; antibacterial and/or antitumor cationic macromolecules; solubilizing agents
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Special Issue Information

Dear Colleagues,

In the last few years, antibiotic resistance and, analogously, anticancer drug resistance have increased considerably, becoming one of the main public health problems needing solutions which can be obtained by finding new therapeutic strategies able to counteract the onset of multi-drug resistance (MDR). Due to several surface similarities between bacteria and cancer cells rather human normal cells, cationic nanosized macromolecules (NPs) mimicking natural antimicrobial peptides (NAMPs) and acting as membrane disruptors have shown potent and selective microbiocidal and anticancer effects and low tendency to develop resistance. Furthermore, water-soluble cationic NPs have proven to be particularly efficient in solubilizing insoluble bioactive small molecules, thus enhancing their bioavailability, activities and promoting their further development as new therapeutic agents. In this context, topical administration and drug delivery via the skin is a convenient and novel approach which allows to avoid first-pass metabolism, thus increasing drug bioavailability. It allows the application of drugs to a large area, avoiding gastro-intestinal irritations caused by the medication and improving patient compliance. In this regard, since only small particles can pass through the skin, NPs are particularly suitable to provide topical formulations. Additionally, cross-linked macromolecules capable of providing gels with intrinsic pharmacological effects or enriched with bioactive molecules by their dispersion in water (hydrogels) have been suggested to overcome the problems associated with conventional topical delivery devices. Hydrogels have gained attention owing to their peculiar characteristics, such as swelling in aqueous media, pH and temperature sensitivity, or sensitivity to other stimuli, biocompatibility, and environmental applicability.

This Special Issue aims to supply a platform for research on the development of new antimicrobial and/or anticancer water-soluble NPs or crosslinked macromolecules, starting from their synthesis to their biological evaluation and/or environmental application, going through their characterization. The simultaneous presence of all these aspects in the same study is not mandatory. We welcome papers with a special focus on the formulation of the bioactive macromolecules as hydrogels for cutaneous uses with low cytotoxicity toward mammalian cells.

Dr. Silvana Alfei
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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Keywords

(cationic) antibacterial nanoparticles
(cationic) anticancer nanoparticles
water-soluble bioactive nanoparticles
cross-linked materials (resins)
(cationic) solubilizing macromolecules
swelling polymers
hydrogels formulations
drug delivery systems
environmental application of resins
spectroscopic characterization
rheological experiments
swelling and porosity characteristics
water loss studies
kinetic mathematical models
multivariate analyses (PCA)

Published Papers (8 papers)

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Research

17 pages, 11484 KiB

Open AccessArticle

Optical Polymorphism of Liquid–Crystalline Dispersions of DNA at High Concentrations of Crowding Polymer

by Vladimir N. Morozov, Mikhail A. Klimovich, Anna V. Shibaeva, Olga N. Klimovich, Ekaterina D. Koshevaya, Maria A. Kolyvanova and Vladimir A. Kuzmin

Int. J. Mol. Sci. 2023, 24(14), 11365; https://doi.org/10.3390/ijms241411365 - 12 Jul 2023

Cited by 1 | Viewed by 846

Abstract

Optically active liquid–crystalline dispersions (LCD) of nucleic acids, obtained by polymer- and salt-induced (psi-) condensation, e.g., by mixing of aqueous saline solutions of low molecular weight DNA (≤10⁶ Da) and polyethylene glycol (PEG), possess an outstanding circular dichroism (CD) signal (so-called psi-CD) and are of interest for sensor applications. Typically, such CD signals are observed in PEG content from ≈12.5% to ≈22%. However, in the literature, there are very conflicting data on the existence of psi-CD in DNA LCDs at a higher content of crowding polymer up to 30–40%. In the present work, we demonstrate that, in the range of PEG content in the system above ≈24%, optically polymorphic LCDs can be formed, characterized by both negative and positive psi-CD signals, as well as by ones rather slightly differing from the spectrum of isotropic DNA solution. Such a change in the CD signal is determined by the concentration of the stock solution of PEG used for the preparation of LCDs. We assume that various saturation of polymer chains with water molecules may affect the amount of active water, which in turn leads to a change in the hydration of DNA molecules and their transition from B-form to Z-form. Full article

(This article belongs to the Special Issue Macromolecules and Hydrogel Formulations: Synthesis, Characterization, Pharmacological Effects and Possible Environmental Applications)

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31 pages, 4479 KiB

Open AccessArticle

Dual-Stimuli-Sensitive Smart Hydrogels Containing Magnetic Nanoparticles as Antitumor Local Drug Delivery Systems—Synthesis and Characterization

by Adam Kasiński, Agata Świerczek, Monika Zielińska-Pisklak, Sebastian Kowalczyk, Andrzej Plichta, Anna Zgadzaj, Ewa Oledzka and Marcin Sobczak

Int. J. Mol. Sci. 2023, 24(8), 6906; https://doi.org/10.3390/ijms24086906 - 07 Apr 2023

Cited by 5 | Viewed by 1693

Abstract

The aim of this study was to develop an innovative, dual-stimuli-responsive smart hydrogel local drug delivery system (LDDS), potentially useful as an injectable simultaneous chemotherapy and magnetic hyperthermia (MHT) antitumor treatment device. The hydrogels were based on a biocompatible and biodegradable poly(ε-caprolactone-co-rac-lactide)-b-poly(ethylene glycol)-b-poly(ε-caprolactone-co-rac-lactide) (PCLA-PEG-PCLA, PCLA) triblock copolymer, synthesized via ring-opening polymerization (ROP) in the presence of a zirconium(IV) acetylacetonate (Zr(acac)₄) catalyst. The PCLA copolymers were successfully synthesized and characterized using NMR and GPC techniques. Furthermore, the gel-forming and rheological properties of the resulting hydrogels were thoroughly investigated, and the optimal synthesis conditions were determined. The coprecipitation method was applied to create magnetic iron oxide nanoparticles (MIONs) with a low diameter and a narrow size distribution. The magnetic properties of the MIONs were close to superparamagnetic upon TEM, DLS, and VSM analysis. The particle suspension placed in an alternating magnetic field (AMF) of the appropriate parameters showed a rapid increase in temperature to the values desired for hyperthermia. The MIONs/hydrogel matrices were evaluated for paclitaxel (PTX) release in vitro. The release was prolonged and well controlled, displaying close to zero-order kinetics; the drug release mechanism was found to be anomalous. Furthermore, it was found that the simulated hyperthermia conditions had no effect on the release kinetics. As a result, the synthesized smart hydrogels were discovered to be a promising antitumor LDDS, allowing simultaneous chemotherapy and hyperthermia treatment. Full article

(This article belongs to the Special Issue Macromolecules and Hydrogel Formulations: Synthesis, Characterization, Pharmacological Effects and Possible Environmental Applications)

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21 pages, 12856 KiB

Open AccessArticle

Simultaneous Administration of Bevacizumab with Bee-Pollen Extract-Loaded Hybrid Protein Hydrogel NPs Is a Promising Targeted Strategy against Cancer Cells

by Nemany A. N. Hanafy, Eman Ali Bakr Eltonouby, Elsayed I. Salim, Magdy E. Mahfouz, Stefano Leporatti and Ezar H. Hafez

Int. J. Mol. Sci. 2023, 24(4), 3548; https://doi.org/10.3390/ijms24043548 - 10 Feb 2023

Cited by 4 | Viewed by 2378

Abstract

Bevacizumab (Bev) a humanized monoclonal antibody that fights vascular endothelial growth factor A (VEGF-A). It was the first specifically considered angiogenesis inhibitor and it has now become the normative first-line therapy for advanced non-small-cell lung cancer (NSCLC). In the current study, polyphenolic compounds were isolated from bee pollen (PCIBP) and encapsulated (EPCIBP) inside moieties of hybrid peptide–protein hydrogel nanoparticles in which bovine serum albumin (BSA) was combined with protamine-free sulfate and targeted with folic acid (FA). The apoptotic effects of PCIBP and its encapsulation (EPCIBP) were further investigated using A549 and MCF-7 cell lines, providing significant upregulation of Bax and caspase 3 genes and downregulation of Bcl2, HRAS, and MAPK as well. This effect was synergistically improved in combination with Bev. Our findings may contribute to the use of EPCIBP simultaneously with chemotherapy to strengthen the effectiveness and minimize the required dose. Full article

(This article belongs to the Special Issue Macromolecules and Hydrogel Formulations: Synthesis, Characterization, Pharmacological Effects and Possible Environmental Applications)

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33 pages, 8486 KiB

Open AccessArticle

Cationic Polystyrene-Based Hydrogels as Efficient Adsorbents to Remove Methyl Orange and Fluorescein Dye Pollutants from Industrial Wastewater

by Silvana Alfei, Federica Grasso, Valentina Orlandi, Eleonora Russo, Raffaella Boggia and Guendalina Zuccari

Int. J. Mol. Sci. 2023, 24(3), 2948; https://doi.org/10.3390/ijms24032948 - 02 Feb 2023

Cited by 8 | Viewed by 1887

Abstract

Water pollution from dyes is harmful to the environment, plants, animals, and humans and is one of the most widespread problems afflicting people throughout the world. Adsorption is a widely used method to remove contaminants derived from the textile industry, food colorants, printing, and cosmetic manufacturing from water. Here, aiming to develop new low-cost and up-scalable adsorbent materials for anionic dye remediation and water decontamination by electrostatic interactions, two cationic resins (R1 and R2) were prepared. In particular, they were obtained by copolymerizing 4-ammonium methyl and ethyl styrene monomers (M1 and M2) with dimethylacrylamide (DMAA), using N-(2-acryloylamino-ethyl)-acrylamide (AAEA) as cross-linker. Once characterized by several analytical techniques, upon their dispersion in an excess of water, R1 and R2 provided the R1- and R2-based hydrogels (namely R1HG and R2HG) with equilibrium degrees of swelling (EDS) of 900% and 1000% and equilibrium water contents (EWC) of 90 and 91%, respectively. By applying Cross’ rheology equation to the data of R1HG and R2HG’s viscosity vs. shear rate, it was established that both hydrogels are shear thinning fluids with pseudoplastic/Bingham plastic behavior depending on share rate. The equivalents of -NH₃⁺ groups, essential for the electrostatic-based absorbent activity, were estimated by the method of Gaur and Gupta on R1 and R2 and by potentiometric titrations on R1HG and R2HG. In absorption experiments in bulk, R1HG and R2HG showed high removal efficiency (97–100%) towards methyl orange (MO) azo dye, fluorescein (F), and their mixture (MOF). Using F or MO solutions (pH = 7.5, room temperature), the maximum absorption was 47.8 mg/g in 90′ (F) and 47.7 mg/g in 120′ (MO) for R1, while that of R2 was 49.0 mg/g in 20′ (F) and 48.5 mg/g in 30′ (MO). Additionally, R1HG and R2HG-based columns, mimicking decontamination systems by filtration, were capable of removing MO, F, and MOF from water with a 100% removal efficiency, in different conditions of use. R1HG and R2HG represent low-cost and up-scalable column packing materials that are promising for application in industrial wastewater treatment. Full article

(This article belongs to the Special Issue Macromolecules and Hydrogel Formulations: Synthesis, Characterization, Pharmacological Effects and Possible Environmental Applications)

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14 pages, 3351 KiB

Open AccessArticle

Portable Alkaline Phosphatase–Hydrogel Platform: From Enzyme Characterization to Phosphate Sensing

by Yolanda Alacid, María José Martínez-Tomé, Rocío Esquembre, M. Antonia Herrero and C. Reyes Mateo

Int. J. Mol. Sci. 2023, 24(3), 2672; https://doi.org/10.3390/ijms24032672 - 31 Jan 2023

Cited by 2 | Viewed by 1687

Abstract

Here, we present a study on the incorporation and characterization of the enzyme alkaline phosphatase (ALP) into a three-dimensional polymeric network through a green protocol to obtain transparent hydrogels (ALP@AETA) that can be stored at room temperature and potentially used as a disposable biosensor platform for the rapid detection of ALP inhibitors. For this purpose, different strategies for the immobilization of ALP in the hydrogel were examined and the properties of the new material, compared to the hydrogel in the absence of enzyme, were studied. The conformation and stability of the immobilized enzyme were characterized by monitoring the changes in its intrinsic fluorescence as a function of temperature, in order to study the unfolding/folding process inside the hydrogel, inherently related to the enzyme activity. The results show that the immobilized enzyme retains its activity, slightly increases its thermal stability and can be stored as a xerogel at room temperature without losing its properties. A small portion of a few millimeters of ALP@AETA xerogel was sufficient to perform enzymatic activity inhibition assays, so as a proof of concept, the device was tested as a portable optical biosensor for the detection of phosphate in water with satisfactory results. Given the good stability of the ALP@AETA xerogel and the interesting applications of ALP, not only in the environmental field but also as a therapeutic enzyme, we believe that this study could be of great use for the development of new devices for sensing and protein delivery. Full article

(This article belongs to the Special Issue Macromolecules and Hydrogel Formulations: Synthesis, Characterization, Pharmacological Effects and Possible Environmental Applications)

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22 pages, 6410 KiB

Open AccessArticle

Biodegradable Guar-Gum-Based Super-Porous Matrices for Gastroretentive Controlled Drug Release in the Treatment of Helicobacter pylori: A Proof of Concept

by Roberto Grosso, Elena Benito, Ana I. Carbajo-Gordillo, M. Gracia García-Martín, Víctor Perez-Puyana, Pablo Sánchez-Cid and M.-Violante de-Paz

Int. J. Mol. Sci. 2023, 24(3), 2281; https://doi.org/10.3390/ijms24032281 - 23 Jan 2023

Cited by 3 | Viewed by 1834

Abstract

An increase in resistance to key antibiotics has made the need for novel treatments for the gastric colonization of Helicobacter pylori (H. pylori) a matter of the utmost urgency. Recent studies tackling this topic have focused either on the discovery of new compounds to ameliorate therapeutic regimes (such as vonoprazan) or the synthesis of gastroretentive drug delivery systems (GRDDSs) to improve the pharmacokinetics of oral formulations. The use of semi-interpenetrating polymer networks (semi-IPNs) that can act as super-porous hydrogels for this purpose is proposed in the present work, specifically those displaying low ecological footprint, easy synthesis, self-floating properties, high encapsulation efficiency for drugs such as amoxicillin (AMOX), great mucoadhesiveness, and optimal mechanical strength when exposed to stomach-like fluids. To achieve such systems, biodegradable synthetic copolymers containing acid-labile monomers were prepared and interpenetrated with guar gum (GG) in a one-pot polymerization process based on thiol-ene click reactions. The resulting matrices were characterized by SEM, GPC, TGA, NMR, and rheology studies, and the acidic hydrolysis of the acid-sensitive polymers was also studied. Results confirm that some of the obtained matrices are expected to perform optimally as GRDDSs for the sustained release of active pharmaceutical ingredients at the gastrointestinal level, being a priori facilitated by its disaggregation. Therefore, the optimal performance of these systems is assessed by varying the molar ratio of the labile monomer in the matrices. Full article

(This article belongs to the Special Issue Macromolecules and Hydrogel Formulations: Synthesis, Characterization, Pharmacological Effects and Possible Environmental Applications)

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24 pages, 7252 KiB

Open AccessArticle

Sodium Alginate-g-acrylamide/acrylic Acid Hydrogels Obtained by Electron Beam Irradiation for Soil Conditioning

by Elena Manaila, Gabriela Craciun and Ion Cosmin Calina

Int. J. Mol. Sci. 2023, 24(1), 104; https://doi.org/10.3390/ijms24010104 - 21 Dec 2022

Cited by 2 | Viewed by 2134

Abstract

Being both a cause and a victim of water scarcity and nutrient deficiency, agriculture as a sustainable livelihood is dependent now on finding new suport solutions. Biodegradable hydrogels usage as soil conditioners may be one of the most effective solutions for irrigation efficiency improvement, reducing the quantity of soluble fertilizers per crop cycle and combating pathogens, due to their versatility assured by both obtaining method and properties. The first goal of the work was the obtaining by electron beam irradiation and characterization of some Sodium Alginate-g-acrylamide/acrylic Acid hydrogels, the second one being the investigation of their potential use as a soil conditioner by successive experiments of absorption and release of two different aqueous nutrient solutions. Alginate-g-acrylamide/acrylic Acid hydrogels were obtained by electron beam irradiation using the linear accelerator ALID 7 at 5.5 MeV at the irradiation doses of 5 and 6 kGy. For this were prepared monomeric solutions that contained 1 and 2% sodium alginate, acrylamide and acrylic acid in ratios of 1:1 and 1.5:1, respectively, for the obtaining of materials with hybrid properties derived from natural and synthetic components. Physical, chemical, structural and morphological characteristics of the obtained hydrogels were investigated by specific analysis using swelling, diffusion and network studies and Fourier Transform Infrared Spectroscopy and Scanning Electron Microscopy. Four successive absorption and release experiments of some synthetic and natural aqueous solutions with nutrients were performed. Full article

(This article belongs to the Special Issue Macromolecules and Hydrogel Formulations: Synthesis, Characterization, Pharmacological Effects and Possible Environmental Applications)

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25 pages, 5551 KiB

Open AccessArticle

A Self-Forming Hydrogel from a Bactericidal Copolymer: Synthesis, Characterization, Biological Evaluations and Perspective Applications

by Silvana Alfei, Alessia Zorzoli, Danilo Marimpietri, Guendalina Zuccari, Eleonora Russo, Debora Caviglia and Anna Maria Schito

Int. J. Mol. Sci. 2022, 23(23), 15092; https://doi.org/10.3390/ijms232315092 - 01 Dec 2022

Cited by 2 | Viewed by 1019

Abstract

Objects touched by patients and healthcare workers in hospitals may harbor pathogens, including multi-drug resistant (MDR) staphylococci, enterococci (VRE), Escherichia coli, Acinetobacter, and Pseudomonas species. Medical devices contaminated by these pathogens may also act as a source of severe and difficult-to-treat human infections, thus becoming a critical public health concern requiring urgent resolutions. To this end, we recently reported the bactericidal effects of a cationic copolymer (CP1). Here, aiming at developing a bactericidal formulation possibly to be used either for surfaces disinfection or to treat skin infections, CP1 was formulated as a hydrogel (CP1_1.1-Hgel). Importantly, even if not cross-linked, CP1 formed the gel upon simple dispersion in water, without requiring gelling agents or other additives which could be skin-incompatible or interfere with CP1 bactericidal effects in possible future topical applications. CP1_1.1-Hgel was characterized by attenuated-total-reflectance Fourier transform infrared (ATR-FTIR) and UV-Vis spectroscopy, as well as optic and scanning electron microscopy (OM and SEM) to investigate its chemical structure and morphology. Its stability was assessed by monitoring its inversion properties over time at room temperature, while its mechanical characteristics were assessed by rheological experiments. Dose-dependent cytotoxicity studies performed on human fibroblasts for 24 h with gel samples obtained by diluting CP_1.1-Hgel at properly selected concentrations established that the 3D network formation did not significantly affect the cytotoxic profile of CP1. Also, microbiologic investigations carried out on two-fold serial dilutions of CP1-gel confirmed the minimum inhibitory concentrations (MICs) previously reported for the not formulated CP1.Selectivity indices values up to 12 were estimated by the values of LD₅₀ and MICs determined here on gel samples. Full article

(This article belongs to the Special Issue Macromolecules and Hydrogel Formulations: Synthesis, Characterization, Pharmacological Effects and Possible Environmental Applications)

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