Search

In light of the increasing resistance of pathogenic microorganisms to the action of antibiotics, essential oils extracted from plants with therapeutic activity provide a significant alternative to obtaining dressings for the treatment of skin wounds. The encapsulation of essential oils in an amphiphilic gel network allows better dispersion and preservation of hydrophobic bioactive substances while promoting their prolonged release. In this study, we focused on the development of a poly (vinyl alcohol) (PVA)/poly (ethylene brassylate-co-squaric acid) (PEBSA) platform embedded with thymol (Thy), and α-tocopherol (α-Tcp) as a co-drug structure with prospective use for the treatment and healing of skin wounds. The new complex bioactive system was prepared through repeated freeze–thaw processes. The influence of the composition on surface topography, hydrophilic/hydrophobic character, and in vitro interaction with simulated body fluids was evidenced. BALB/3T3 fibroblast cell culture demonstrated the cryogel scaffolds’ cytocompatibility. Tests on Wistar rats confirmed their biocompatibility, integration with host tissue, and the absence of inflammatory processes. The bioactive compound significantly enhanced the healing process of full-thickness excision wounds in a rat model. Further investigations on in vivo infection models would assess the potential of the PVA/PEBSA platform with dual bioactive activity for clinical antimicrobial and wound healing therapy.

The interactions between poly(acrylic acid) (PAA), poly(vinyl alcohol) (PVA), and lysozyme (Lys) in an aqueous environment at pHs of 2, 4, and 7.4 were discussed considering the experimental data obtained by turbidimetry, electrokinetic and rheological measurements, and FTIR analysis. It was found that the increase in PAA amount reduces the coacervation zone by shifting the critical pHcr1to higher values while the critical pHcr2 remains unchanged. The coacervation zone extended from 3.1–4.2 to 2.9–4.7 increasing the Lys concentration from 0.2% to 0.5%. The zeta potential measurements showed that the PAA–PVA–Lys mixture in water is the most stable in the pH range of 4.5–8. Zero shear viscosity exhibited deviations from additivity at both investigated pHs, and a maximum value corresponding to a maximum hydrodynamic volume was revealed at PAA weight fractions of 0.4 and 0.5 for pHs of 4 and 7.4, respectively. The binding affinity to Lys of PAA, established by molecular dynamics simulation, was slightly higher than that of PVA. The more stable complex was PAA–Lys formed in a very acidic environment; for that, a binding affinity of −7.1 kcal/mol was determined.

Meloxicam (MX) is a nonsteroidal anti-inflammatory drug (NSAID) used mainly to reduce pain, inflammation, and fever. In the present study, thermosensitive polyurethane (PU)-based hydrogels with various excipients (PEG, PVP, HPC, and essential oil) were prepared and loaded with MX. Rheological investigations were carried out on the PU-based formulations in various shear regimes, and their viscoelastic characteristics were determined. The average size of the PU micelles was 35.8 nm at 37 °C and slightly increased at 37 nm in the presence of MX. The zeta potential values of the hydrogels were between −10 mV and −11.5 mV. At pH = 6 and temperature of 37 °C, the formulated PU-based hydrogels loaded with MX could deliver significant amounts of the active substance, between 60% and 80% over 24–48 h and more than 90% within 2 weeks. It was found that anomalous transport phenomena dominated MX’s release mechanism from the PU-based networks. The results are encouraging for further studies aiming to design alternative carriers to commercial dosage forms of nonsteroidal anti-inflammatory drugs.

The evaluation of the properties and characteristics of macromolecular compounds is essential, especially from the point of view of the potential uses of the studied compounds. In this regard, poly(ethylene brassylate-co-squaric acid) (PEBSA) copolymacrolactone was investigated in order to correlate the relationships between the structure of the compounds and the generated properties. The study evaluates the physicochemical characteristics of PEBSA in interdependence with the ratio between comonomers, namely ethylene brassylate (EB) and squaric acid (SA), and the extent to which the structural tunability of the polymers generated by the SA content affects the properties in terms of the thermal stability, dielectric characteristics, and structural properties resulted from X-ray diffraction analysis. A good thermal stability of the copolymers was registered; this behaviour was interdependent with the squaric acid content and attributed to the intermolecular physical bonds achieved through the carbonyl functional groups of SA. The evaluation of the dielectric properties of the copolymers evidenced also the dependence of these characteristics on the SA content. The role of SA in creating self-organized morphologies with specific shapes and sizes was put into evidence by the AFM study. The supramolecular structure of PEBSA induced by the presence of squaric acid through hydrogen bonds interactions and π-stacking was confirmed by the X-ray diffraction. Also, both hydrogen donor and acceptor potential of these copolymers opens increased applicability for these new polymer systems.

The study presents the development of a new copolymacrolactone structure based on ethylene brassylate (EB) and squaric acid (SA) with different ratios between comonomers. The new system was tested as a network for essential oils encapsulation. The structure of the copolymers was confirmed by spectroscopic investigations and correlated in interdependence with the comonomers content. The interfacial characteristics of the poly(ethylene brassylate-co-squaric acid) copolymers were determined, and the transition from a moderate hydrophilic surface towards a hydrophobic region by increasing the molar content of SA comonomer was highlighted. The affinity for hydrophobic substances of the synthesised macromolecular compounds was used in a process of encapsulation of thymol (Thy) and carvacrol (CC). The newly prepared bioactive compounds were characterised by in vivo biocompatibility tests, and antimicrobial activity, Minimum Inhibitory Concentration (MIC) and Minimum Bactericidal Concentration (MBC).

The study presents the possibility of covering Ag nanoparticles in solutuon with cellulose with cellulose nanofibrils (CNFs)and oxidized cellulose nanofibrils, termed TEMPO (TCNFs)in order to increase their dispersility and stability over time. The chemical composition of the prepared hybrid complexes was confirmed by FTIR spectroscopy. DLS investigation highlighted the increased stability in time of AgNPs after their covering with cellulose nanofibrils derivatives. Moreover, good results were obtained after covering the AgNPs in solution with TCNFs, a phenomenon explained by the presence of carboxylic groups (introduced during the TEMPO compound formation) capable of supplementary/ additional physical bonds establishment. Optical microscopy images of the hybrid solutions deposited on microscope slides evidenced the modification of the surface morphology films and attested the silver nanoparticle presence. Thus, while the increase of the dispersive stability of AgNPs is achieved, an antimicrobial chaeacter for the cellulose nanofibrils is acquired.

The inability to meet and ensure as many requirements as possible is fully justified by the continuous interest in obtaining new multifunctional materials. A new cryogel system based on poly(vinyl alcohol) (PVA) and poly(ethylene brassylate-co-squaric acid) (PEBSA) obtained by repeated freeze–thaw processes was previously reported and used for the incorporation of an antibacterial essential oil—namely, thymol (Thy). Furthermore, the present study aims to confer antioxidant properties to the PVA/PEBSA_Thy system by encapsulating α-tocopherol (α-Tcp), targeting a double therapeutic effect due to the presence of both bioactive compounds. The amphiphilic nature of the PEBSA copolymer allowed for the encapsulation of both Thy and α-Tcp, via an in situ entrapment method. The new PVA/PEBSA_Thy_α-Tcp systems were characterized in terms of their influence on the composition, network morphology and release profiles, as well as their antimicrobial and antioxidant properties. The study underlined the cumulative antioxidant efficiency of Thy and α-Tcp, which in combination with the PEBSA copolymer have a synergistic effect (97.1%). We believe that the convenient and simple strategy offered in this study increases applicability for these new PVA/PEBSA_Thy_α-Tcp cryogel systems.

Development of natural protein-based hydrogels with self-healing performance and tunable physical properties has attracted increased attention owing to their wide potential not only in the pharmaceutical field, but also in wounds management. This work reports the development of a versatile hydrogel based on enzymatically-crosslinked gelatin and nanogels loaded with amoxicillin (Amox), an antibiotic used in wound infections. The transglutaminase (TGase)-crosslinked hydrogels and encapsulating nanogels were formed rapidly through enzymatic crosslinking and self-assembly interactions in mild conditions. The nanogels formed through the self-assemble of maleoyl-chitosan (MAC5) and polyaspartic acid (PAS) may have positive influence on the self-healing capacity and drug distribution within the hydrogel network through the interactions established between gelatin and gel-like nanocarriers. The physicochemical properties of the enzymatically-crosslinked hydrogels, such as internal structure, swelling and degradation behavior, were studied. In addition, the Amox release studies indicated a rapid release when the pH of the medium decreased, which represents a favorable characteristic for use in the healing of infected wounds. It was further observed through the in vitro and in vivo biocompatibility assays that the optimized scaffolds have great potential to be used as wound dressings.

Double network (DN) hydrogels composed of self-assembling low-molecular-weight gelators and a hybrid polymer network are of particular interest for many emerging biomedical applications, such as tissue regeneration and drug delivery. The major benefits of these structures are their distinct mechanical properties as well as their ability to mimic the hierarchical features of the extracellular matrix. Herein, we describe a hybrid synthetic/natural polymer gel that acts as the initial network based on sodium alginate and a copolymer, namely poly(itaconic anhydride-co-3,9-divinyl-2,4,8,10-tetraoxaspiro (5,5) undecane). The addition of amino acids and peptide-derived hydrogelators, such as Fmoc-Lys-Fmoc-OH and Fmoc-Gly-Gly-Gly-OH, to the already-made network gives rise to DNs crosslinked via non-covalent interactions. Fourier transform infrared spectroscopy (FTIR) and thermal analysis confirmed the formation of the DN and highlighted the interactions between the two component networks. Swelling studies revealed that the materials have an excellent water absorption capacity and can be classified as superabsorbent gels. The rheological properties were systematically investigated in response to different variables and showed that the prepared materials present injectability and a self-healing ability. SEM analysis revealed a morphology consisting of a highly porous and interconnected fibrous network. Finally, the biocompatibility was evaluated using the MTT assay on dermal fibroblasts, and the results indicated that the new structures are non-toxic and potentially useful for biomedical applications.

The study presents the achievement of a new assembly with antioxidant behaviour based on a copolymacrolactone structure that encapsulates erythritol (Eryt). Poly(ethylene brassylate-co-squaric acid) (PEBSA) was synthesised in environmentally friendly conditions, respectively, through a process in suspension in water by opening the cycle of ethylene brassylate macrolactone, followed by condensation with squaric acid. The compound synthesised in suspension was characterised by comparison with the polymer obtained by polymerisation in solution. The investigations revealed that, with the exception of the molecular masses, the compounds generated by the two synthetic procedures present similar properties, including good thermal stability, with a Tpeak of 456 °C, and the capacity for network formation. In addition, the investigation by dynamic light scattering techniques evidenced a mean diameter for PEBSA particles of around 596 nm and a zeta potential of −25 mV, which attests to their stability. The bio-based copolymacrolactone was used as a matrix for erythritol encapsulation. The new PEBSA–Eryt compound presented an increased sorption/desorption process, compared with the PEBSA matrix, and a crystalline morphology confirmed by X-ray diffraction analysis. The bioactive compound was also characterised in terms of its biocompatibility and antioxidant behaviour.

Hydrogels based on natural, biodegradable materials have gained considerable interest in the medical field due to their improved drug delivery profiles and tissue-mimicking architecture. In this regard, this study was devoted to the preparation and characterization of new physically crosslinked hydrogels based on carboxymethyl cellulose and an unconventional crosslinking agent, phytic acid. Phytic acid, in addition to its antioxidant and antibacterial effects, can improve the biological properties and stability of gels, without adding toxicity. Fourier transform infrared (FTIR) spectroscopy, rheological studies and thermal analysis confirmed the hydrogel formation. The influence of the ratio between the cellulose derivative and the crosslinker upon the morphological structure and water uptake was evidenced by scanning electron microscopy (SEM) and swelling measurements in simulated body fluids. Furthermore, procaine was entrapped within the hydrogels and used as a model drug for in vitro studies, which highlighted the dependence of the drug release on the phytic acid content of the matrix. The materials demonstrated antibacterial effects against Escherichia coli and Staphylococcus aureus bacteria. The biocompatibility was assessed on fibroblast cells, and according to our results, hydrogels can improve cell viability highlighting the potential of these systems as therapeutic scaffolds for skin tissue engineering.

One of the methods of obtaining supramolecular gels consists of the possibility of self-assembly of low molecular weight gelators (LMWGs). However, LMWG-based gels are often difficult to handle, easy to destroy and have poor rheological performance. In order to improve the gels’ properties, the LMWGs molecules are co-assembled, which induces more cross-links with more stable structures. Starting from these aspects, the present study refers to the preparation of a bionic hydrogel stabilized with a physiologically occurring, bifunctional biomolecule, L-lysine, co-assembled with other amino acids or peptides (such as a modified amino acid (Fmoc-serine or Fmoc-glutamic acid) or a tripeptide (Fmoc-Gly-Gly-Gly)) with the potential to support the repair of injuries or the age-related impaired structures or functions of living tissues. The introduction of a copartner aims to improve hydrogel characteristics from a morphological, rheological and structural point of view. On the other hand, the process will allow the understanding of the phenomenon of specific self-association and molecular recognition. Various characterization techniques were used to assess the ability to co-assemble: DLS, FT-IR, SEM and fluorescence microscopy, rheology and thermal analysis. Studies have confirmed that the supramolecular structure occurs through the formation of inter- and intramolecular physical bonds that ensure the formation of fibrils organized into 3D networks. The rheological data, namely the G′ > G″ and tan δ approximately 0.1–0.2 gel-like behavior observed for all studied samples, demonstrate and sustain the appearance of the co-assembly processes and the ability of the samples to act as LMWG. From the studied systems, the Fmoc–Lys–Fmoc_ Fmoc–Glu sample presented the best rheological characteristics that are consistent with the observations that resulted from the dichroism, fluorescence and SEM investigations.

Physical cryogels were obtained using the successive freeze–thaw technique of poly(vinyl alcohol) (PVA)/poly(ethylene brassylate-co-squaric acid) (PEBSA) solutions. The cryogel systems were prepared by using two different molecular weights of PVA and PEBSA with three different ratios between the ethylene brassylate (EB) and squaric acid (SA) comonomers. The presence of interactions, the thermal properties and the morphology were investigated using Fourier Transform Infrared Spectroscopy (FT-IR), thermogravimetry (TGA and DTG) and scanning electron microscopy (SEM), respectively. The influence of the composition on the degree of swelling in a physiological environment was demonstrated. The study highlighted improvements in terms of new network flexibility due to the intermolecular chains interactions brought by the introduction of PEBSA in the cryogel structure. We also concluded that the presence of PEBSA in the PVA/PEBSA cryogel network improved the loading capacity of the new system with specific hydrophobic agents, for example essential oils, which (due to their antimicrobial character) can lead to the use of new systems obtained for various applications.

Squaric acid (SA) is a compound with potential to crosslink biomacromolecules. Although SA has become over the last years a well-known crosslinking agent as a result of its good biocompatibility, glutaraldehyde (GA), a compound with proven cytotoxicity is still one of the most used crosslinkers to develop nanomaterials. In this regard, the novelty of the present study consists in determining whether it may be possible to substitute GA with a new bifunctional and biocompatible compound, such as SA, in the process of enzyme immobilization on the surface of magnetic nanoparticles (MNPs). Thus, a direct comparison between SA- and GA-functionalized magnetic nanoparticles was realized in terms of physico-chemical properties and ability to immobilize catalytic enzymes. The optimal conditions of the synthesis of the two types of GOx-immobilized MNPs were described, thus emphasizing the difference between the two reagents. Scanning Electron Microscopy and Dynamic Light Scattering were used for size, shape and colloidal stability characterization of the pristine MNPs and of those coupled with GOx. Binding of GOx to MNPs by using GA or SA was confirmed by FT-IR spectroscopy. The stability of the immobilized and free enzyme was investigated by measuring the enzymatic activity. The study confirmed that the resulting activity of the immobilized enzyme and the optimization of enzyme immobilization depended on the type of reagent used and duration of the process. The catalytic performance of immobilized enzyme was tested, revealing that the long-term colloidal stability of SA-functionalized MNPs was superior to those prepared with GA. In conclusion, the SA-functionalized bioconjugates have a better potential as compared to the GA-modified nanosystems to be regarded as catalytic nanodevices for biomedical purposes such as biosensors.

This study reports a strategy for developing a biohybrid complex based on a natural/synthetic polymer conjugate as a gel-type structure. Coupling synthetic polymers with natural compounds represents an important approach to generating gels with superior properties and with potential for biomedical applications. The study presents the preparation of hybrid gels with tunable characteristics by using a spiroacetal polymer and alginate as co-partners in different ratios. The new network formation was tested, and the structure was confirmed by FTIR and SEM techniques. The physical properties of the new gels, namely their thermal stability and swelling behavior, were investigated. The study showed that the increase in alginate content caused a smooth increase in thermal stability due to the additional crosslinking bridges that appeared. Moreover, increasing the content of the synthetic polymer in the structure of the gel network ensures a slower release of carvacrol, the encapsulated bioactive compound.

Nanogels in biomedical field are promising and innovative materials as dispersions of hydrogel nanoparticles based on crosslinked polymeric networks that have been called as next generation drug delivery systems due to their relatively high drug encapsulation capacity, uniformity, tunable size, ease of preparation, minimal toxicity, stability in the presence of serum, and stimuli responsiveness. Nanogels show a great potential in chemotherapy, diagnosis, organ targeting and delivery of bioactive substances. The main subjects reviewed in this article concentrates on: (i) Nanogel assimilation in the nanomedicine domain; (ii) Features and advantages of nanogels, the main characteristics, such as: swelling capacity, stimuli sensitivity, the great surface area, functionalization, bioconjugation and encapsulation of bioactive substances, which are taken into account in designing the structures according to the application; some data on the advantages and limitations of the preparation techniques; (iii) Recent progress in nanogels as a carrier of genetic material, protein and vaccine. The majority of the scientific literature presents the multivalency potential of bioconjugated nanogels in various conditions. Today’s research focuses over the overcoming of the restrictions imposed by cost, some medical requirements and technological issues, for nanogels’ commercial scale production and their integration as a new platform in biomedicine.

Bio-based compounds are a leading direction in the context of the increased demand for these materials due to the numerous advantages associated with their use over conventional materials, which hardly degrade in the environment. At the same time, the use of essential oils and their components is generated mainly by finding alternative solutions to antibiotics and synthetic preservatives due to their bioactive characteristics, but also to their synergistic capacity during the manifestation of different biological properties. The present study is devoted to poly(ethylene brassylate-co-squaric acid) (PEBSA), synthesis and its use for thymol encapsulation and antibacterial system formation. The synthesized copolymer, performed through ethylene brassylate macrolactone ring-opening and copolymerization with squaric acid, was physicochemical characterized. Its amphiphilic character allowed the entrapment of thymol (Ty), a natural monoterpenoid phenol found in oil of thyme, a compound with strong antiseptic properties. The copolymer chemical structure was confirmed by spectroscopic analyses. Thermal analysis evidenced a good thermal stability for the copolymer. Additionally, the antimicrobial activity of PEBSA_Ty complex was investigated against eight different reference strains namely: bacterial strains—Staphylococcus aureus ATCC25923, Escherichia coli ATCC25922, Enterococcus faecalis ATCC 29212, Klebsiella pneumonie ATCC 10031 and Salmonella typhimurium ATCC 14028, yeast strains represented by Candida albicans ATCC10231 and Candida glabrata ATCC 2001, and the fungal strain Aspergillus brasiliensis ATCC9642.

Protein-polysaccharide systems are of increasing interest as their combined attributes allow for fulfilling a broad range of applications in biomedical and pharmaceutical fields. In this study, the preparation of nanogels based on maleic anhydride chitosan derivatives (MAC) and bovine serum albumin (BSA) was achieved through a self-assembly process performed in aqueous phase. A series of experiments performed by varying the concentrations of MAC and BSA were conducted to find an appropriate mixing ratio for the polymer solutions leading to thermodynamically stable nanogels with the ability to encapsulate active compounds. The influence of temperature on the formation of nanogels was also studied. The consequent conformational changes were monitored using ultraviolet-visible (UV-VIS) spectrophotometry. The spectrophotometric investigations combined with diffraction light scattering (DLS) technique and zeta potential measurement results were correlated to determine the interaction mechanism and assess the self-assembling processes during nanogel formation. It was found that the hydrodynamic diameter (Dh) of the nanoparticles increased slightly at acidic pH, and the protonation of ionizable amino groups with the pH was confirmed by the zeta potential measurements. MAC/BSA nanogels also exhibited antimicrobial properties after being loaded with amoxicillin (Amox), which is an antibiotic used for the treatment of various infections. The experimental data resulting from this study provide theoretical guidance for the design and development of attractive nanocarriers for a large variety of biomedical applications.

(1) Background: The fascinating properties of currently synthesized aerogels associated with the flexible approach of sol-gel chemistry play an important role in the emergence of special biomedical applications. Although it is increasingly known and mentioned, the potential of aerogels in the medical field is not sufficiently explored. Interest in aerogels has increased greatly in recent decades due to their special properties, such as high surface area, excellent thermal and acoustic properties, low density and thermal conductivity, high porosity, flame resistance and humidity, and low refractive index and dielectric constant. On the other hand, high manufacturing costs and poor mechanical strength limit the growth of the market. (2) Results: In this paper, we analyze more than 180 articles from recent literature studies focused on the dynamics of aerogels research to summarize the technologies used in manufacturing and the properties of materials based on natural polymers from renewable sources. Biomedical applications of these bio-based materials are also introduced. (3) Conclusions: Due to their complementary functionalities (bioactivity, biocompatibility, biodegradability, and unique chemistry), bio-based materials provide a vast capability for utilization in the field of interdisciplinary and multidisciplinary scientific research.

In the present study polyelectrolyte complexes (PECs) based on new sulfadiazine-chitosan conjugates with sodium hyaluronate have been developed with potential use in treatment of burn wounds. The PECs were chemically characterized using Fourier Transform—Infrared Spectroscopy, Scanning Electon Microscopy and Near Infrared Chemical Imaging Technique. The swelling behavior and in vitro sulfadiazine release were also investigated. The antimicrobial activity was evaluated towards three bacterial strains: Escherichia coli, Listeria monocytogenes and Salmonella thyphymurium. The developed PECs demonstrated their antimicrobial efficiency against tested bacterial strains, the PECs containing sulfadiazine-modified chitosan being more active than PECs containing unmodified chitosan.