Biomolecule-Based Supramolecular Hydrogels for Biomedical Applications: The Current Trends

A special issue of Pharmaceutics (ISSN 1999-4923). This special issue belongs to the section "Biologics and Biosimilars".

Deadline for manuscript submissions: closed (20 June 2023) | Viewed by 9542

Special Issue Editors


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Guest Editor
ChemBioPharm, ARN: Régulations Naturelle et Artificielle, Université de Bordeaux, INSERM U1212, CNRS UMR 5320, ARNA, 33076 Bordeaux, France
Interests: hydrogel; supramolecular self-assembly; drug delivery system; low-molecular-weight gelator; physico-chemical characterization; pharmaceutical development

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Guest Editor
ChemBioPharm, ARN: Régulations Naturelle et Artificielle, Université de Bordeaux, INSERM U1212, CNRS UMR 5320, ARNA, 33076 Bordeaux, France
Interests: modified oligonucleotides; nucleic acid bioconjugates for multiple applications; ranging from molecular building blocks for self-assemblies to biomedical and therapeutic applications
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Special Issue Information

Dear Colleagues,

The past few years were very profusive in the field of hydrogels, especially for biomedical applications. Even if a majority of the research focused on polymeric hydrogels, the supramolecular ones, and more especially those that are biomolecule-based, aroused much interest. Indeed, their structures, composed of nucleic acids, saccharides, proteins, peptides, etc., increase their biocompatibility, widening their potential applications. Their ability to encapsulate active substances, their responsiveness to stimuli, and their self-assembling and mechanical properties are real strengths for numerous systems, such as nano/micro hydrogels, scaffolds for tissue engineering, bioink, etc.

This Special Issue will focus on original papers and reviews on the current trends in biomolecule-based supramolecular hydrogels. Such matrices, owing to their versatility and intrinsic characteristics, are real assets for biomedical applications, i.e., drug delivery systems, cell culture scaffolds, and 3D bioprinting. To have an overview of the novelties in this field, subjects ranging from the design of biomolecule-based gelators, their formulation, and their physico-chemical characterization to their in vitro and in vivo evaluation will be developed.

We wish to dedicate this Special Issue to the memory of our colleague and friend, Dr. Laurent Latxague.

Prof. Dr. Alexandra Gaubert
Prof. Dr. Philippe Barthélémy
Guest Editors

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Keywords

  • biomolecule-based hydrogels
  • supramolecular self-assembly
  • biomedical applications
  • drug delivery systems
  • cell culture matrix
  • low-molecular-weight gelators
  • peptide
  • nucleic acid
  • protein
  • saccharide

Published Papers (5 papers)

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Research

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25 pages, 8611 KiB  
Article
Lignin–Cobalt Nano-Enabled Poly(pseudo)rotaxane Supramolecular Hydrogel for Treating Chronic Wounds
by Giulia Crivello, Giuliana Orlandini, Angela Gala Morena, Alessandro Torchio, Clara Mattu, Monica Boffito, Tzanko Tzanov and Gianluca Ciardelli
Pharmaceutics 2023, 15(6), 1717; https://doi.org/10.3390/pharmaceutics15061717 - 13 Jun 2023
Cited by 2 | Viewed by 1188
Abstract
Chronic wounds (CWs) are a growing issue for the health care system. Their treatment requires a synergic approach to reduce both inflammation and the bacterial burden. In this work, a promising system for treating CWs was developed, comprising cobalt-lignin nanoparticles (NPs) embedded in [...] Read more.
Chronic wounds (CWs) are a growing issue for the health care system. Their treatment requires a synergic approach to reduce both inflammation and the bacterial burden. In this work, a promising system for treating CWs was developed, comprising cobalt-lignin nanoparticles (NPs) embedded in a supramolecular (SM) hydrogel. First, NPs were obtained through cobalt reduction with phenolated lignin, and their antibacterial properties were tested against both Gram-negative and Gram-positive strains. The anti-inflammatory capacity of the NPs was proven through their ability to inhibit myeloperoxidase (MPO) and matrix metalloproteases (MMPs), which are enzymes involved in the inflammatory process and wound chronicity. Then, the NPs were loaded in an SM hydrogel based on a blend of α-cyclodextrin and custom-made poly(ether urethane)s. The nano-enabled hydrogel showed injectability, self-healing properties, and linear release of the loaded cargo. Moreover, the SM hydrogel’s characteristics were optimized to absorb proteins when in contact with liquid, suggesting its capacity to uptake harmful enzymes from the wound exudate. These results render the developed multifunctional SM material an interesting candidate for the management of CWs. Full article
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16 pages, 5116 KiB  
Article
Mineralization of Bone Extracellular Matrix-like Scaffolds Fabricated as Silk Sericin-Functionalized Dense Collagen–Fibrin Hybrid Hydrogels
by Gabriele Griffanti, Marc D. McKee and Showan N. Nazhat
Pharmaceutics 2023, 15(4), 1087; https://doi.org/10.3390/pharmaceutics15041087 - 28 Mar 2023
Cited by 3 | Viewed by 1992
Abstract
The design of hydrogels that combine both the biochemical cues needed to direct seeded cellular functions and mineralization to provide the structural and mechanical properties approaching those of mineralized native bone extracellular matrix (ECM) represents a significant challenge in bone tissue engineering. While [...] Read more.
The design of hydrogels that combine both the biochemical cues needed to direct seeded cellular functions and mineralization to provide the structural and mechanical properties approaching those of mineralized native bone extracellular matrix (ECM) represents a significant challenge in bone tissue engineering. While fibrous hydrogels constituting of collagen or fibrin (and their hybrids) can be considered as scaffolds that mimic to some degree native bone ECM, their insufficient mechanical properties limit their application. In the present study, an automated gel aspiration–ejection (automated GAE) method was used to generate collagen–fibrin hybrid gel scaffolds with micro-architectures and mechanical properties approaching those of native bone ECM. Moreover, the functionalization of these hybrid scaffolds with negatively charged silk sericin accelerated their mineralization under acellular conditions in simulated body fluid and modulated the proliferation and osteoblastic differentiation of seeded MC3T3-E1 pre-osteoblastic cells. In the latter case, alkaline phosphatase activity measurements indicated that the hybrid gel scaffolds with seeded cells showed accelerated osteoblastic differentiation, which in turn led to increased matrix mineralization. In summary, the design of dense collagen–fibrin hybrid gels through an automated GAE process can provide a route to tailoring specific biochemical and mechanical properties to different types of bone ECM-like scaffolds, and can provide a model to better understand cell–matrix interactions in vitro for bioengineering purposes. Full article
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21 pages, 5024 KiB  
Article
Pluronic® F127 Thermoresponsive Viscum album Hydrogel: Physicochemical Features and Cellular In Vitro Evaluation
by Mariana S. Rocha, João V. C. Batista, Michelle N. O. Melo, Vania E. B. de Campos, Anna Lecticia M. M. Toledo, Adriana P. Oliveira, Paulo H. S. Picciani, Stephan Baumgartner and Carla Holandino
Pharmaceutics 2022, 14(12), 2775; https://doi.org/10.3390/pharmaceutics14122775 - 12 Dec 2022
Cited by 4 | Viewed by 1794
Abstract
Viscum album L., popularly known as mistletoe, is well known for its anti-cancer properties, and the pharmaceutical application of hydroalcoholic dry extracts is still limited due to its low solubility in aqueous media, and physicochemical instability. The Pluronic® F127 is an amphiphilic [...] Read more.
Viscum album L., popularly known as mistletoe, is well known for its anti-cancer properties, and the pharmaceutical application of hydroalcoholic dry extracts is still limited due to its low solubility in aqueous media, and physicochemical instability. The Pluronic® F127 is an amphiphilic polymer, which permits the solubilization of lipophilic and hydrophilic compounds. In this investigation, physicochemical features of hydrogel containing V. album dry extract (VADE-loaded-hydrogel) were performed by: dynamic light scattering (DLS), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), and transmission electron microscopy (TEM). VADE-loaded-hydrogel presented nanometer-size micelles with volume distribution ranging from 10.58 nm to 246.7 nm, and a polydispersity index of 0.441. The sample thermal analyses (TG and DSC) showed similar decomposition curves; however, the thermal events indicated an increase in thermal stability in relation to the presence of the extract. In addition to these interesting pharmaceutical features, IC50 values of 333.40 µg/mL and >1000 µg/mL were obtained when tumor (SCC-25) and non-tumor (L929) cells were incubated with VADE-loaded-hydrogel, respectively. The optical and ultrastructural cellular analysis confirmed the tumor selectivity since the following alterations were detected only in SCC-25 cells: disorganization of plasmatic membrane; an increase of cytoplasmatic vacuole size; alteration in the cristae mitochondrial shape; and generation of amorphous cellular material. These results emphasize the promising antitumoral potential of VADE-loaded-hydrogel as an herbal drug delivery system via in vitro assays. Full article
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15 pages, 4093 KiB  
Article
Smart Injectable Chitosan Hydrogels Loaded with 5-Fluorouracil for the Treatment of Breast Cancer
by Ahmed A. H. Abdellatif, Ahmed M. Mohammed, Imran Saleem, Mansour Alsharidah, Osamah Al Rugaie, Fatma Ahmed and Shaaban K. Osman
Pharmaceutics 2022, 14(3), 661; https://doi.org/10.3390/pharmaceutics14030661 - 17 Mar 2022
Cited by 19 | Viewed by 2721
Abstract
The treatment of breast cancer requires long chemotherapy management, which is accompanied by severe side effects. Localized delivery of anticancer drugs helps to increase the drug concentration at the site of action and overcome such a problem. In the present study, chitosan hydrogel [...] Read more.
The treatment of breast cancer requires long chemotherapy management, which is accompanied by severe side effects. Localized delivery of anticancer drugs helps to increase the drug concentration at the site of action and overcome such a problem. In the present study, chitosan hydrogel was prepared for local delivery of 5-Fluorouracil. The in vitro release behavior was investigated and the anticancer activity was evaluated against MCF-7 cells using MTT assay. The in vivo studies were investigated via intra-tumoral injection of a 5-FU loaded hydrogel into breast cancer of female rats. The results indicated that the modified hydrogel has excellent physicochemical properties with a sustained in vitro release profile matching a zero-order kinetic for one month. In addition, the hydrogel showed superior inhibition of cell viability compared with the untreated control group. Moreover, the in vivo studies resulted in antitumor activity with minor side effects. The tumor volume and level of tumor markers in blood were inhibited significantly by applying the hydrogel compared with the untreated control group. In conclusion, the designed injectable hydrogels are potential drug delivery systems for the treatment of breast cancer with a controlled drug release profile, which could be suitable for decreasing the side effects of chemotherapy agents. Full article
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Review

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24 pages, 7058 KiB  
Review
Chitosan-Based Particulate Carriers: Structure, Production and Corresponding Controlled Release
by Jiaqi Weng, Alain Durand and Stéphane Desobry
Pharmaceutics 2023, 15(5), 1455; https://doi.org/10.3390/pharmaceutics15051455 - 10 May 2023
Cited by 4 | Viewed by 1105
Abstract
The state of the art in the use of chitosan (CS) for preparing particulate carriers for drug delivery applications is reviewed. After evidencing the scientific and commercial potentials of CS, the links between targeted controlled activity, the preparation process and the kinetics of [...] Read more.
The state of the art in the use of chitosan (CS) for preparing particulate carriers for drug delivery applications is reviewed. After evidencing the scientific and commercial potentials of CS, the links between targeted controlled activity, the preparation process and the kinetics of release are detailed, focusing on two types of particulate carriers: matrix particles and capsules. More precisely, the relationship between the size/structure of CS-based particles as multifunctional delivery systems and drug release kinetics (models) is emphasized. The preparation method and conditions greatly influence particle structure and size, which affect release properties. Various techniques available for characterizing particle structural properties and size distribution are reviewed. CS particulate carriers with different structures can achieve various release patterns, including zero-order, multi-pulsed, and pulse-triggered. Mathematical models have an unavoidable role in understanding release mechanisms and their interrelationships. Moreover, models help identify the key structural characteristics, thus saving experimental time. Furthermore, by investigating the close relation between preparation process parameters and particulate structural characteristics as well as their effect on release properties, a novel “on-demand” strategy for the design of drug delivery devices may be developed. This reverse strategy involves designing the production process and the related particles’ structure based on the targeted release pattern. Full article
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