Advanced hydrogels based on natural macromolecules: chemical routes to achieve mechanical versatility

abstract

Advances in synthetic routes to chemically modify natural macromolecules such as polysaccharides and proteins have allowed designing functional hydrogels able to tackle current challenges in the biomedical field. Hydrogels are hydrophilic three-dimensional systems able to absorb or retain a large volume of water, prepared from a low percentage of precursor macromolecules. The typical fragile elastic structure of common hydrogel formulations often limits their usage. Three main fabrication strategies involving several compounds or multimodified materials known as double networks, dual-crosslinked networks, and interpenetrating networks have been explored to impart mechanical strength to hydrogels. Widely investigated for synthetic polymers, these approaches allow obtaining added-value hydrogels with a large spectrum of mechanical properties. Advances in the development of such hydrogels with bio-macromolecules as main constituent materials have enabled the fabrication of hydrogels with improved key properties for medical use, including biocompatibility, controlled release of active substances and tailored biodegradability, while exploring sustainable sources. This review describes recent advances in the use of proteins, as well as natural and semi-synthetic polymers for the fabrication of hydrogels for biomedical applications. Structures processed via double network, dual-crosslinked, or interpenetrating network strategies are reviewed, and emphasis is given to the type of chemical modifications and re-actions, as well as the covalent and non-covalent interactions/bonds involved in those mechanisms.(c) 2022 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

keywords

DOUBLE-NETWORK HYDROGELS; AZIDE-ALKYNE CYCLOADDITION; CARBOXYMETHYL CELLULOSE HYDROGELS; HYALURONIC-ACID HYDROGELS; WOUND-HEALING PROPERTIES; FREE CLICK CHEMISTRY; CROSS-LINKING; IN-SITU; SUPRAMOLECULAR HYDROGEL; TANNIC-ACID

subject category

Chemistry; Materials Science

authors

Mortier, C; Costa, DCS; Oliveira, MB; Haugen, HJ; Lyngstadaas, SP; Blaker, JJ; Mano, JF

Groups

G5 - Biomimetic, Biological and Living Materials

Projects

Human Platelet Lysates-based Scaffolds for Interfacial Multi-tissue Repair (INTERLYNK)

A bioactivated nano-layered hydrogel for dermal regeneration in hard-to-heal ulcers (BioNaNor)

CICECO - Aveiro Institute of Materials (UIDB/50011/2020)

CICECO - Aveiro Institute of Materials (UIDP/50011/2020)

Associated Laboratory CICECO-Aveiro Institute of Materials (LA/P/0006/2020)

Desenvolvimento de hidrogeis de inspiracao marinha multifuncionais e de elevado desempenho para regeneracao de cartilagem, reticulados com ligacoes nao-covalentes e bio-instrutivas deslizantes. (MARGEL)

acknowledgements

The authors would like to acknowledge the support of the European Union (EU) Horizon 2020 for the project InterLynk, grant agreement: H2020-NMBP-TR-IND-2020, project ID: 953169. This work was supported by the project A Bioactivated Nano-layered Hydrogel for Dermal Regeneration in Hard-to-Heal Ulcers(Bio-NaNOR) financed by Research Council of Norway (RCN) Nano2021: grant number 287991. This work was also developed within the scope of the project CICECO-Aveiro Institute of Materials, UIDB/50011/2020, UIDP/50011/2020 and LA/P/0006/2020, financed by national funds through the FCT/MEC (PIDDAC) This work was also supported by the Programa Operacional Competitividade e Internacionalizacao (POCI) , in the component FEDER, and by national funds (OE) through FCT/MCTES in the scope of the project MARGEL (PTDC/BTM-MAT/31498/2017) . The MARGEL project is acknowledged for the individual Junior Researcher contract of Dora C. S. Costa, and M. B. Oliveira knowledges the individual Assistant Researcher contract 2021.03588.CEECIND.